In this work, the propylene glycol monomethyl ether (PGME) + dimethyl sulfoxide (DMSO) system was used in absorption process of SO 2 , and the gas−liquid equilibrium (GLE) data of SO 2 in the PGME + DMSO system were determined at T = 298.15, 303.15, and 308.15 K and p = 123.15 kPa. The experimental data are used to develop SO 2 solubility model, which shows a potential application for SO 2 removal. After that, Henry's law constants (HLCs) were calculated by fitting the linear slope of solubility, and thermodynamic parameters were computed on the basis of the correlation of HLCs. The regeneration experimental results showed that 98.5% SO 2 can be desorbed at 333.15 K and N 2 bubbling in 12 min, and no significant loss of absorption capacity for absorption solvents. Additionally, FTIR, UV−vis, and 1 H NMR spectra were recorded to discuss the interaction between SO 2 and the binary systems of PGME + DMSO, and the results indicated that intermolecular hydrogen bonding association among PGME, DMSO, and SO 2 was formed.