A bis(uranyl) complex (phen)(UO2)(μ2–F)(F)]2 (A) and its solvated form A?·?(H2O)n were examined using scalar relativistic density functional theory. Hydrogen bonds cause the phen ligand to slightly deviate from the equatorial plane of the uranyl ion, resulting in a pronounced red-shift of the U–F-terminal and U?=?O asymmetric stretching vibrations. The calculated energies fall within 4.4?–6.8 kcal/mol. Explicit and/or implicit aqueous solvation re-arranges the molecular orbitals of the complex