Reactions of laser-ablated U atoms with SO2 Molecules gave the very stable U(VI) molecule, SUO2, as the major product. Infrared absorptions for two new O=U=O stretching modes were observed in solid argon and neon. The band assignments were confirmed by appropriate (SO2)-S-34, (SO2)-O-18, and (SO2)-O-16,18 isotopic shifts. B3LYP and BPW91 density functional calculations were performed to determine molecular structure, vibrational frequencies, and isotopic shifts. The C-2v structure is analogous to those computed for UO3 and US3. Minor products were identified as SUO, the SUO2+ cation, and the (SO2)(SUO2) adduct.