Siloxides can support U! in the reduction of small molecules with uranium complexes. The treatment of [UN(SiMe3)23] with HOSi(OtBu)3 (3 equiv) yielded a novel homoleptic uranium(III) siloxide complex 1, which acted as a two-electron reducing agent toward CS 2 and CO2 (see scheme). Complex 1 also reduced toluene to afford a diuranium inverted-sandwich complex. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.