Uranium(V)-imido-iodide complexes have been prepared by chemical oxidation of the corresponding uranium(IV)-imido complexes with copper(I) iodide. These U(V) organometallic systems show reversible U-V/U-IV and U-VI/U-V redox behavior in addition to classic 50 spectroscopic signatures. The generality of this Cu(I)-based oxidation protocol is demonstrated by preparation of the analogous U(V)imido-triflate and -thiolate complexes using CuOTf and CuSPh, respectively.