Reduction of IU(NHAriPr6)(2) (Ar-iPr6 = 2,6-(2,4,6-(Pr3C6H2)-Pr-i)(2)C6H3) results in a rare example of a U(II) complex, U(NHAriPr6)(2), and the first example that is a neutral species. Here, we show spectroscopic and magnetic studies that suggest a 5f(4)6d(0) valence electronic configuration for uranium, along with characterization of related U(III) complexes.