Laser-ablated U atoms react with discharged sulfur vapor in excess argon to form the US, US2, and US3 Molecules, which are identified from matrix infrared spectra using sulfur isotopic substitution, Vibrational frequencies from quasi relativistic DFT calculations support these assignments and provide an insight into the bonding and structure. Unlike linear UO2, US2 is bent because of more favorable U(6d)-S(3p) overlap, and US2 has a 118 +/- 5degrees (experimental based on isotopic shift) or 121degrees (calculated B-3(2) ground state, B3LYP) S-U-S bond angle.