Building on our report that collision-induced dissociation (CID) can be used to create the highly reactive U-alkylidyne species O=U≡CH , our goal was to determine whether the species could be as an intermediate for synthesis of OUS by reaction with carbon disulfide (CS ). Cationic uranyl-propiolate precursor ions were generated by electrospray ionization, and multiple-stage CID in a linear trap instrument was used to prepare O=U≡CH . Neutral CS was admitted into the trap through a modified He inlet and precision leak valves. The O=U≡CH ion reacts with CS to generate OUS . CID of OUS causes elimination of the axial sulfide ligand to generate OU . Using isotopically labeled reagent, we found that OUS reacts with O to create UO . O=U≡CH proves to be a useful reagent ion for synthesis of OUS , a species that to date has only been created by gas-phase reactions of U and U . Dissociation of OUS to create OU , but not US , and the efficient conversion of the species into UO , is consistent with the relative differences in U-O and U-S bond energies.