High‐Performance and Breathable Polypyrrole Coated Air‐Laid Paper for Flexible All‐Solid‐State Supercapacitors

High‐performance, breathable, conductive, and flexible polypyrrole (PPy) coated paper electrodes are prepared by an interfacial polymerization method using air‐laid paper as a substrate. Owing to the synergistic effect of superior electrical conductivity, high wettability, and the porous architecture, the prepared electrode not only shows an outstanding specific capacitance and rate abilities (3100 and 2579 mF cm^?2 at 1 and 20 mA cm^?2 for a PPy coated paper electrode), but also exhibits excellent flexibility, wearability, and breathability. Based on these superior features, an all‐solid‐state supercapacitor assembled with the PPy coated paper electrodes shows an outstanding energy density of 62.4 µW h cm^?2, remarkable air permeability and excellent flexibility to sustain various deformations. Furthermore, large‐scale fabrication of conductive flexible paper electrode can be easily achieved through this method. Therefore, this work offers a new vision for flexible energy storage.     

Conductive Metal–Organic Frameworks Selectively Grown on Laser‐Scribed Graphene for Electrochemical Microsupercapacitors

Conductive 2D metal–organic frameworks (MOFs) have merits beyond traditional MOFs for electrochemical applications, but reports on using MOFs as electrodes for electrochemical microsupercapacitors (MSCs) are practically non‐existent. In this work, a Ni‐catecholate‐based MOF (Ni‐CAT MOF) having good conductivity and exhibiting redox chemistry in the positive and negative voltage windows is developed. A novel process is developed to selectively grow the conductive Ni‐CAT MOF on 3D laser scribed graphene (LSG). The LSG with its superior wettability serves as a functional matrix‐current collector for the hybridization of conductive Ni‐CAT MOF nanocrystals. Impressively, MSCs fabricated using the hybrid LSG/Ni‐CAT MOF show significant improvement compared with MOF‐free LSG electrodes. Specifically, the LSG/Ni‐CAT MOF electrodes can deliver MSCs with a wide operating voltage (1.4 V), high areal capacitance (15.2 mF cm^?2), energy density (4.1 µWh cm^?2), power density (7 mW cm^?2), good rate performance, and decent cycling stability. This work opens up an avenue for developing electrochemical microsupercapacitors using conductive MOF electrodes.     

All‐Printed MnHCF‐MnOx‐Based High‐Performance Flexible Supercapacitors

Here, a simple active materials synthesis method is presented that boosts electrode performance and utilizes a facile screen‐printing technique to prepare scalable patterned flexible supercapacitors based on manganese hexacyanoferrate‐manganese oxide and electrochemically reduced graphene oxide electrode materials (MnHCF‐MnO_x/ErGO). A very simple in situ self‐reaction method is developed to introduce MnO_x pseudocapacitor material into the MnHCF system by using NH₄F. This MnHCF‐MnO_x electrode materials can deliver excellent capacitance of 467 F g^?1 at a current density of 1 A g^?1, which is a 2.4 times capacitance increase compared to MnHCF. In addition a printed, patterned, flexible MnHCF‐MnO_x/ErGO supercapacitor is fabricated, showing a remarkable areal capacitance of 16.8 mF cm^?2 and considerable energy and power density of 0.5 mWh cm^?2 and 0.0023 mW cm^?2, respectively. Furthermore, the printed patterned flexible supercapacitors also exhibit exceptional flexibility, and the capacitance remains stable, even while bending to various angles (60°, 90°, and 180°) and for 100 cycles. The flexible supercapacitor arrays integrated by multiple prepared single supercapacitors can power various LEDs even in the bent states. This approach offers promising opportunities for the development of printable energy storage materials and devices with high energy density, large scalability, and excellent flexibility.     

3D,Mutually Embedded MOF@Carbon Nanotube Hybrid Networks for High‐Performance Lithium‐Sulfur Batteries

Metal‐organic frameworks (MOFs) hybridized with a conductive matrix could potentially serve as a sulfur host for lithium‐sulfur (Li‐S) battery electrodes; so far most of the previously studied hybrid structures are in the powder form or thin compact films. This study reports 3D porous MOF@carbon nanotube (CNT) networks by grafting MOFs with tailored particle size uniformly throughout a CNT sponge skeleton. Growing larger‐size MOF particles to entrap the conductive CNT network yields a mutually embedded structure with high stability, and after sulfur encapsulation, it shows an initial discharge capacity of ≈1380 mA h g^?1 (at 0.1 C) and excellent cycling stability with a very low fading rate. Furthermore, owing to the 3D porous network that is suitable for enhanced sulfur loading, a remarkable areal capacity of ≈11 mA h cm^?2 (at 0.1 C) is obtained, which is much higher than other MOF‐based hybrid electrodes. The mutually embedded MOF@CNTs with simultaneously high specific capacity, areal capacity, and cycling stability represent an advanced candidate for developing high‐performance Li‐S batteries and other energy storage systems.     

Highly Flexible,Freestanding Supercapacitor Electrode with Enhanced Performance Obtained by Hybridizing Polypyrrole Chains with MXene

Though polypyrrole (PPy) is widely used in flexible supercapacitors owing to its high electrochemical activity and intrinsic flexibility, limited capacitance and cycling stability of freestanding PPy films greatly reduce their practicality in real‐world applications. Herein, we report a new approach to enhance PPy's capacitance and cycling stability by forming a freestanding and conductive hybrid film through intercalating PPy into layered Ti₃C₂ (l‐Ti₃C₂, a MXene material). The capacitance increases from 150 (300) to 203 mF cm^?2 (406 F cm^?3). Moreover, almost 100% capacitance retention is achieved, even after 20 000 charging/discharging cycles. The analyses reveal that l‐Ti₃C₂ effectively prevents dense PPy stacking, benefiting the electrolyte infiltration. Furthermore, strong bonds, formed between the PPy backbones and surfaces of l‐Ti₃C₂, not only ensure good conductivity and provide precise pathways for charge‐carrier transport but also improve the structural stability of PPy backbones. The freestanding PPy/l‐Ti₃C₂ film is further used to fabricate an ultra‐thin all‐solid‐state supercapacitor, which shows an excellent capacitance (35 mF cm^?2), stable performance at any bending state and during 10 000 charging/discharging cycles. This novel strategy provides a new way to design conductive polymer‐based freestanding flexible electrodes with greatly improved electrochemical performances.     

Paper‐Based Energy‐Storage Devices Comprising Carbon Fiber‐Reinforced Polypyrrole‐Cladophora Nanocellulose Composite Electrodes

Composites of polypyrrole (PPy) and Cladophora nanocellulose, reinforced with 8 μm‐thick chopped carbon filaments, can be used as electrode materials to obtain paper‐based energy‐storage devices with unprecedented performance at high charge and discharge rates. Charge capacities of more than 200 C g^?1 (PPy) are obtained for paper‐based electrodes at potential scan rates as high as 500 mV s^?1, whereas cell capacitances of ～60–70 F g^?1 (PPy) are reached for symmetric supercapacitor cells with capacitances up to 3.0 F (i.e.,0.48 F cm^?2) when charged to 0.6 V using current densities as high as 31 A g^?1 based on the PPy weight (i.e., 99 mA cm^?2). Energy and power densities of 1.75 Wh kg^?1 and 2.7 kW kg^?1, respectively, are obtained when normalized with respect to twice the PPy weight of the smaller electrode. No loss in cell capacitance is seen during charging/discharging at 7.7 A g^?1 (PPy) over 1500 cycles. It is proposed that the nonelectroactive carbon filaments decrease the contact resistances and the resistance of the reduced PPy composite. The present straightforward approach represents significant progress in the development of low‐cost and environmentally friendly paper‐based energy‐storage devices for high‐power applications.     

Inverted Design for High‐Performance Supercapacitor Via Co(OH)2‐Derived Highly Oriented MOF Electrodes

Metal organic frameworks (MOFs) are considered as promising candidates for supercapacitors because of high specific area and potential redox sites. However, their shuffled orientations and low conductivity nature lead to severely‐degraded performance. Designing an accessibly‐manipulated and efficient method to address those issues is of outmost significance for MOF application in supercapacitors. It is the common way that MOFs scarify themselves as templates or precursors to prepare target products. But to reversely think it, using target products to prepare MOF could be the way to unlock the bottleneck of MOFs' performance in supercapacitors. Herein, a novel strategy using Co(OH)₂ as both the template and precursor to fabricate vertically‐oriented MOF electrode is proposed. The electrode shows a double high specific capacitance of 1044 Fg^?1 and excellent rate capability compared to MOF in powder form. An asymmetric supercapacitor was also fabricated, which delivers a maximum energy density of 28.5 W h kg^?1 at a power density of 1500 W kg^?1, and the maximum of 24000 W kg^?1 can be obtained with a remaining energy density of 13.3 W h kg^?1. Therefore, the proposed strategy paves the way to unlock the inherent advantages of MOFs and also inspires for advanced MOF synthesis with optimum performance.     

High Performance,Flexible, Solid‐State Supercapacitors Based on a Renewable and Biodegradable Mesoporous Cellulose Membrane

A flexible, transparent, and renewable mesoporous cellulose membrane (mCel‐membrane) featuring uniform mesopores of ≈24.7 nm and high porosity of 71.78% is prepared via a facile and scalable solution‐phase inversion process. KOH‐saturated mCel‐membrane as a polymer electrolyte demonstrates a high electrolyte retention of 451.2 wt%, a high ionic conductivity of 0.325 S cm^?1, and excellent mechanical flexibility and robustness. A solid‐state electric double layer capacitor (EDLC) using activated carbon as electrodes, the KOH‐saturated mCel‐membrane as a polymer electrolyte exhibits a high capacitance of 110 F g^?1 at 1.0 A g^?1, and long cycling life of 10 000 cycles with 84.7% capacitance retention. Moreover, a highly integrated planar‐type micro‐supercapacitor (MSC) can be facilely fabricated by directly depositing the electrode materials on the mCel‐membrane‐based polymer electrolyte without using complicated devices. The resulting MSC exhibits a high areal capacitance of 153.34 mF cm^?2 and volumetric capacitance of 191.66 F cm^?3 at 10 mV s^?1, representing one of the highest values among all carbon‐based MSC devices. These findings suggest that the developed renewable, flexible, mesoporous cellulose membrane holds great promise in the practical applications of flexible, solid‐state, portable energy storage devices that are not limited to supercapacitors.     

Graphitic Petal Electrodes for All‐Solid‐State Flexible Supercapacitors

The charge storage characteristics of a composite nanoarchitecture with a highly functional 3D morphology are reported. The electrodes are formed by the electropolymerization of aniline monomers into a nanometer‐thick polyaniline (PANI) film that conformally coats graphitic petals (GPs) grown by microwave plasma chemical vapor deposition (MPCVD) on conductive carbon cloth (CC). The hybrid CC/GPs/PANI electrodes yield results near the theoretical maximum capacitance for PANI of 2000 F g^?1 (based on PANI mass) and a large area‐normalized specific capacitance of ≈2.6 F cm^?2 (equivalent to a volumetric capacitance of ≈230 F cm^?3) at a low current density of 1 A g^?1 (based on PANI mass). The specific capacitances remain above 1200 F g^?1 (based on PANI mass) for currents up to 100 A g^?1 with correspondingly high area‐normalized values. The hybrid electrodes also exhibit a high rate capability with an energy density of 110 Wh kg^?1 and a maximum power density of 265 kW kg^?1 at a current density of 100 A g^?1. Long‐term cyclic stability is good (≈7% loss of initial capacitance after 2000 cycles), with coulombic efficiencies >99%. Moreover, prototype all‐solid‐state flexible supercapacitors fabricated from these hybrid electrodes exhibit excellent energy storage performance.     

3D‐Printed Stretchable Micro‐Supercapacitor with Remarkable Areal Performance

While stretchable micro‐supercapacitors (MSCs) have been realized, they have suffered from limited areal electrochemical performance, thus greatly restricting their practical electronic application. Herein, a facile strategy of 3D printing and unidirectional freezing of a pseudoplastic nanocomposite gel composed of Ti₃C₂T_x MXene nanosheets, manganese dioxide nanowire, silver nanowires, and fullerene to construct intrinsically stretchable MSCs with thick and honeycomb‐like porous interdigitated electrodes is introduced. The unique architecture utilizes thick electrodes and a 3D porous conductive scaffold in conjunction with interacting material properties to achieve higher loading of active materials, larger interfacial area, and faster ion transport for significantly improved areal energy and power density. Moreover, the oriented cellular scaffold with fullerene‐induced slippage cell wall structure prompts the printed electrode to withstand large deformations without breaking or exhibiting obvious performance degradation. When imbued with a polymer gel electrolyte, the 3D‐printed MSC achieves an unprecedented areal capacitance of 216.2 mF cm^?2 at a scan rate of 10 mV s^?1, and remains stable when stretched up to 50% and after 1000 stretch/release cycles. This intrinsically stretchable MSC also exhibits high rate capability and outstanding areal energy density of 19.2 µWh cm^?2 and power density of 58.3 mW cm^?2, outperforming all reported stretchable MSCs.     

Graphene–Cellulose Paper Flexible Supercapacitors

A simple and scalable method to fabricate graphene‐cellulose paper (GCP) membranes is reported; these membranes exhibit great advantages as freestanding and binder‐free electrodes for flexible supercapacitors. The GCP electrode consists of a unique three‐dimensional interwoven structure of graphene nanosheets and cellulose fibers and has excellent mechanical flexibility, good specific capacitance and power performance, and excellent cyclic stability. The electrical conductivity of the GCP membrane shows high stability with a decrease of only 6% after being bent 1000 times. This flexible GCP electrode has a high capacitance per geometric area of 81 mF cm^?2, which is equivalent to a gravimetric capacitance of 120 F g^?1 of graphene, and retains >99% capacitance over 5000 cycles. Several types of flexible GCP‐based polymer supercapacitors with various architectures are assembled to meet the power‐energy requirements of typical flexible or printable electronics. Under highly flexible conditions, the supercapacitors show a high capacitance per geometric area of 46 mF cm^?2 for the complete devices. All the results demonstrate that polymer supercapacitors made using GCP membranes are versatile and may be used for flexible and portable micropower devices.     

Utilizing Waste Cable Wires for High‐Performance Fiber‐Based Hybrid Supercapacitors: An Effective Approach to Electronic‐Waste Management

In recent years, electronic waste (e‐waste) such as old cable wires, fans, circuit boards, etc., can be often seen in large piles of leftover in dumping yards. Employing these e‐waste sources for energy storage devices not only increases the economic value but also decreases the reliance on fossil fuels. In this context, waste cable wires are utilized to obtain precious copper (Cu) fibers and used as a cost‐effective current collector for the fabrication of fiber‐based hybrid supercapacitor (FHSC). With the braided Cu fibers, forest‐like nickel oxide nanosheet grafted carbon nanotube coupled copper oxide nanowire arrays (NiO NSs@CNTs@CuO NWAs/Cu fibers) are designed via simple wet‐chemical approaches. As a battery‐type material, the forest‐like NiO NSs@CNTs@CuO NWAs/Cu fiber electrode shows superior electrochemical properties including high specific capacity (230.48 mA h g^?1) and cycling stability (82.72%) in aqueous alkaline electrolyte. Moreover, a solid‐state FHSC is also fabricated using forest‐like NiO NSs@CNTs@CuO NWAs/Cu fibers as a positive electrode and activated carbon coated carbon fibers as a negative electrode with a gel electrolyte, which also shows a higher energy and power densities of 26.32 W h kg^?1 and 1218.33 W kg^?1, respectively. The flexible FHSC is further employed as an energy source for various electronic gadgets, demonstrating its suitability for wearable applications.     

Wearable High‐Performance Supercapacitors Based on Silver‐Sputtered Textiles with FeCo2S4–NiCo2S4 Composite Nanotube‐Built Multitripod Architectures as Advanced Flexible Electrodes

To achieve high‐performance wearable supercapacitors (SCs), a new class of flexible electrodes with favorable architectures allowing large porosity, high conductivity, and good mechanical stability is strongly needed. Here, this study reports the rational design and fabrication of a novel flexible electrode with nanotube‐built multitripod architectures of ternary metal sulfides' composites (FeCo₂S₄–NiCo₂S₄) on a silver‐sputtered textile cloth. Silver sputtering is applicable to almost all kinds of textiles, and S^2? concentration is optimized during sulfidation process to achieve such architectures and also a complete sulfidation assuring high conductivity. New insights into concentration‐dependent sulfidation mechanism are proposed. The additive‐free FeCo₂S₄–NiCo₂S₄ electrode shows a high specific capacitance of 1519 F g^?1 at 5 mA cm^?2 and superior rate capability (85.1% capacitance retention at 40 mA cm^?2). All‐solid‐state SCs employing these advanced electrodes deliver high energy density of 46 W h kg^?1 at 1070 W kg^?1 as well as achieve remarkable cycling stability retaining 92% of initial capacitance after 3000 cycles at 10 mA cm^?2, and outstanding reliability with no capacitance degradation under large twisting. These are attributed to the components' synergy assuring rich redox reactions, high conductivity as well as highly porous but robust architectures. An almost linear increase in capacitance with devices' area indicates possibility to meet various energy output requirements. This work provides a general, low‐cost route to wearable power sources.     

Flexible and High‐Loading Lithium–Sulfur Batteries Enabled by Integrated Three‐In‐One Fibrous Membranes

Lithium–sulfur batteries are appealing as high‐energy storage systems and hold great application prospects in wearable and portable electronics. However, severe shuttle effects, low sulfur conductivity, and especially poor electrode mechanical flexibility restrict sulfur utilization and loading for practical applications. Herein, high‐flux, flexible, electrospun fibrous membranes are developed, which succeed in integrating three functional units (cathode, interlayer, and separator) into an efficient composite. This structure helps to eliminate negative interface effects, and effectively drives synergistic boosts to polysulfide confinement, electron transfer, and lithium‐ion diffusion. It delivers a high initial capacity of 1501 mA h g^?1 and a discharge capacity of 933 mA h g^?1 after 400 cycles, with slow capacity attenuation (0.069% per cycle). Even under high sulfur loading (13.2 mg cm^?2, electrolyte/sulfur ratio = 6 mL g^?1) or in an alternative folded state, this three‐in‐one membrane still exhibits high areal capacity (11.4 mA h cm^?2) and exceptional application performance (powering an array of over 30 light‐emitting diodes (LEDs)), highlighting its huge potential in high‐energy flexible devices.     

Boron Element Nanowires Electrode for Supercapacitors

The pursuit of new categories of active materials as electrodes of supercapacitors remains a great challenge. Herein, for the first time, elemental boron as a superior electrode material of supercapacitors is reported, which exhibits significantly high capacitances and excellent rate performance in all alkaline, neutral, and acidic electrolytes. Notably, boron nanowire‐carbon fiber cloth (BNWs‐CFC) electrodes achieve a capacitance up to 42.8 mF cm^?2 at a scan rate of 5 mV s^?1 and 60.2 mF cm^?2 at a current density of 0.2 mA cm^?2 in the acidic electrolyte. Moreover, in all these three kinds of electrolytes, BNWs‐CFC electrodes demonstrate a decent cycling stability with >80% capacitance retention after 8000 charging/discharging cycles. The Dominating energy storage mechanism of BNWs in the different electrolytes is analyzed by looking into the kinetics of the electrochemical process. Subsequently, the BNWs‐CFC electrode is used to fabricate a flexible solid‐state supercapacitor, which reveals a specific capacitance up to 22.73 mF cm^?2 and good mechanical performance after 1000 bending cycles. This study opens a new avenue to explore elemental boron‐based new nanomaterials for the application of energy storage with superior electrochemical performance.     

Hydrous RuO2‐Decorated MXene Coordinating with Silver Nanowire Inks Enabling Fully Printed Micro‐Supercapacitors with Extraordinary Volumetric Performance

The fabrication of fully printable, flexible micro‐supercapacitors (MSCs) with high energy and power density remains a significant technological hurdle. To overcome this grand challenge, the 2D material MXene has garnered significant attention for its application, among others, as a printable electrode material for high performing electrochemical energy storage devices. Herein, a facile and in situ process is proposed to homogeneously anchor hydrous ruthenium oxide (RuO₂) nanoparticles on Ti₃C₂T_x MXene nanosheets. The resulting RuO₂@MXene nanosheets can associate with silver nanowires (AgNWs) to serve as a printable electrode with micrometer‐scale resolution for high performing, fully printed MSCs. In this printed nanocomposite electrode, the RuO₂ nanoparticles contribute high pseudocapacitance while preventing the MXene nanosheets from restacking, ensuring an effective ion highway for electrolyte ions. The AgNWs coordinate with the RuO₂@MXene to guarantee the rheological property of the electrode ink, and provide a highly conductive network architecture for rapid charge transport. As a result, MSCs printed from the nanocomposite inks demonstrate volumetric capacitances of 864.2 F cm^?3 at 1 mV s^?1, long‐term cycling performance (90% retention after 10 000 cycles), good rate capability (304.0 F cm^?3 at 2000 mV s^?1), outstanding flexibility, remarkable energy (13.5 mWh cm^?3) and power density (48.5 W cm^?3).     

Scalable Water‐Based Production of Highly Conductive 2D Nanosheets with Ultrahigh Volumetric Capacitance and Rate Capability

Highly conductive and ultrathin 2D nanosheets are of importance for the development of portable electronics and electric vehicles. However, scalable production and rational design for highly electronic and ionic conductive 2D nanosheets still remain a challenge. Herein, an industrially adoptable fluid dynamic exfoliation process is reported to produce large quantities of ionic liquid (IL)‐functionalized metallic phase MoS₂ (m‐MoS₂) and defect‐free graphene (Gr) sheets. Hybrid 2D–2D layered films are also fabricated by incorporating Gr sheets into compact m‐MoS₂ films. The incorporated IL functionalities and Gr sheets prevent aggregation and restacking of the m‐MoS₂ sheets, thereby creating efficient and rapid ion and electron pathways in the hybrid films. The hybrid film with a high packing density of 2.02 g cm^?3 has an outstanding volumetric capacitance of 1430.5 F cm^?3 at 1 A g^?1 and an extremely high rate capability of 80% retention at 1000 A g^?1. The flexible supercapacitor assembled using a polymer‐gel electrolyte exhibits excellent resilience to harsh electrochemical and mechanical conditions while maintaining an impressive rate performance and long cycle life. Successful achievement of an ultrahigh volumetric energy density (1.14 W h cm^?3) using an organic electrolyte with a wide cell voltage of ≈3.5 V is demonstrated.     

Lignin Laser Lithography: A Direct‐Write Method for Fabricating 3D Graphene Electrodes for Microsupercapacitors

In this work, a simple lignin‐based laser lithography technique is developed and used to fabricate on‐chip microsupercapacitors (MSCs) using 3D graphene electrodes. Specifically, lignin films are transformed directly into 3D laser‐scribed graphene (LSG) electrodes by a simple one‐step CO₂ laser irradiation. This step is followed by a water lift‐off process to remove unexposed lignin, resulting in 3D graphene with the designed electrode patterns. The resulting LSG electrodes are hierarchically porous, electrically conductive (conductivity is up to 66.2 S cm^?1), and have a high specific surface area (338.3 m² g^?1). These characteristics mean that such electrodes can be used directly as MSC electrodes without the need for binders and current collectors. The MSCs fabricated using lignin laser lithography exhibit good electrochemical performances, namely, high areal capacitance (25.1 mF cm^?2), high volumetric energy density (≈1 mWh cm^?3), and high volumetric power density (≈2 W cm^?3). The versatility of lignin laser lithography opens up the opportunity in applications such as on‐chip microsupercapacitors, sensors, and flexible electronics at large‐scale production.     

Flexible Asymmetric Micro‐Supercapacitors Based on Bi2O3 and MnO2 Nanoflowers: Larger Areal Mass Promises Higher Energy Density

A flexible asymmetric supercapacitor (ASC) with high energy density is designed and fabricated using flower‐like Bi₂O₃ and MnO₂ grown on carbon nanofiber (CNF) paper as the negative and positive electrodes, respectively. The lightweight (1.6 mg cm^?2), porous, conductive, and flexible features make the CNF paper an ideal support for guest active materials, which permit a large areal mass of 9 mg cm^?2 for Bi₂O₃ (≈85 wt% of the entire electrode). Thus, the optimal device with an operation voltage of 1.8 V can deliver a high energy density of 43.4 μWh cm^?2 (11.3 W h kg^?1, based on the total electrodes) and a maximum power density of 12.9 mW cm^?2 (3370 W kg^?1). This work provides an example of large areal mass and flexible electrode for ASCs with high areal capacitance and high energy density, holding great promise for future flexible electronic devices.     

A Three‐Dimensionally Interconnected Carbon Nanotube–Conducting Polymer Hydrogel Network for High‐Performance Flexible Battery Electrodes

High‐performance flexible energy‐storage devices have great potential as power sources for wearable electronics. One major limitation to the realization of these applications is the lack of flexible electrodes with excellent mechanical and electrochemical properties. Currently employed batteries and supercapacitors are mainly based on electrodes that are not flexible enough for these purposes. Here, a three‐dimensionally interconnected hybrid hydrogel system based on carbon nanotube (CNT)‐conductive polymer network architecture is reported for high‐performance flexible lithium ion battery electrodes. Unlike previously reported conducting polymers (e.g., polyaniline, polypyrrole, polythiophene), which are mechanically fragile and incompatible with aqueous solution processing, this interpenetrating network of the CNT‐conducting polymer hydrogel exibits good mechanical properties, high conductivity, and facile ion transport, leading to facile electrode kinetics and high strain tolerance during electrode volume change. A high‐rate capability for TiO₂ and high cycling stability for SiNP electrodes are reported. Typically, the flexible TiO₂ electrodes achieved a capacity of 76 mAh g^–1 in 40 s of charge/discharge and a high areal capacity of 2.2 mAh cm^–2 can be obtained for flexible SiNP‐based electrodes at 0.1C rate. This simple yet efficient solution process is promising for the fabrication of a variety of high performance flexible electrodes.