Treating both UI 3 (THF) 4 and UI 4 (dioxane) 2 with one equivalent of potassium hydrotris(3phenylpyrazolyl)borate, KTp Ph , resulted in the formation of new low-valent uranium derivatives, Tp Ph UI 2 (THF) 2 (1) and Tp Ph UI 3 (2), respectively. Spectroscopic characterization of these species shows that the Tp Ph ligand is 1,2-borotropically shifted, causing one phenyl group to point towards the B-H rather than the uranium center. Derivatization of these materials was possible via salt metathesis reactions, and in each case, the borotropically shifted phenyl group is maintained. Treating trivalent 1 with one equivalent of potassium phenoxide, KOPh, afforded trivalent Tp Ph U(OPh)I(THF) 2 (1-OPh), whereas, a uranium(IV) derivative, Tp Ph UI 2 (Phpz)(THF) (2-Phpz), was synthesized by treating 2 with potassium 3-phenylpyrazolide, KPhpz. All compounds were characterized by 1 H and 11 B NMR, infrared, and electronic absorption spectroscopies, and where possible, X-ray crystallography.