Uranium derivatives of a redox-active, dioxo-phenoxazine ligand, (DOPOq)(2)UO2, (DOPOsq)UI2(THF)(2), (DOPOcat)UI(THF)(2), and Cp*U(DOPOcat)(THF)(2) (DOPO = 2,4,6,8-tetra-tert-butyl-1-oxo-1H-phenoxazin-9-olate), have been synthesized from U(VI) and U(III) starting materials. Full characterization of these species show uranium complexes bearing ligands in three different oxidation states. The electronic structures of these complexes have been explored using H-1 NMR and electronic absorption spectroscopies, and where possible, X-ray crystallography and SQUID magnetometry.