In this work, the absorption of sulfur dioxide (SO2) was investigated using the 1,3-propanediol (PDO) + dimethyl sulfoxide (DMSO) system, and the gas−liquid equilibrium (GLE) data were analyzed over a temperature range of 298.15–318.15 K (with a temperature gradient of 5 K) at a pressure of 123.15 kPa. By fitting the gas–liquid equilibrium data, it is observed that the process of absorption SO2 conforms to Henry’s Law. The change in specific entropy, enthalpy, and Gibbs free energies of the SO2 absorption process was as well calculated. In addition, the capture and regeneration properties of the PDO + DMSO system were investigated under atmospheric pressure, and the results of regeneration experiments demonstrated that 97.3% of SO2 could be desorbed by heating and bubbling with N2. Furthermore, there was no notable reduction in absorption capacity of the absorbent solvents after multiple cycles. Finally, the FTIR spectra and computational information were noted to analyze the interaction between SO2 and the system. As a result, an intermolecular hydrogen bonding association between PDO, DMSO, and SO2 can be inferred.