The cyclic voltammogram of [(eta(5)-C2B9H11)(2)UBr2]. 2[Li(THF4)] shows the electrochemical generation of a uranium-(III) species. Subsequent Na/Hg reduction of [(eta(5)-C2B9H11)(2)UBr2]. 2[Li(THF4)] leads to the new isolable uranium(III) species [(eta(5)-C2B9H11)(2)UBr(THF)]. 2[Li(THF)(x)] (x = 2-4). The green uranium(III) complex was characterized by NMR and elemental analysis and its structure determined by single-crystal X-ray crystallography. The coordination geometry around the dinegative uranium(III) moiety is pseudotetrahedral with two dicarbollide ligands, a bromide ligand, and a THF ligand. The electrochemical properties of the dicarbollide complex are discussed and compared to similar cyclopentadienyluranium complexes.