In this work, isothermal gas-liquid equilibrium (GLE) data were measured for dilute SO2 in the binary system N,N-dimethylformamide (DMF) (1) + diethylene glycol (DEG) (2) at T = (298.15, 303.15, 313.15, and 318.15) K and p = 122.66 kPa. Based on the GLE data, Henry's law constants were obtained by fitting the linear slope of GLE data, and the thermodynamic parameters were calculated. The thermodynamic results showed that the dissolving processes of dilute SO2 in the binary system are spontaneous, enthalpy driving, and reversible behavior. When conventional UV, FT-IR, and H-1 NMR spectroscopic techniques were used for inspection of spectral changes of dilute SO2 in the binary system DMF (1) + DEG (2), the spectral results suggest that hydrogen bonding and interaction of carbonyl oxygen atoms in DMF with hydroxyl hydrogen atoms in DEG were formed as HC=O center dot center dot center dot HO-CH2CH2-O-CH2CH2-OH center dot center dot center dot, and the strong absorption capability of SO2 in the binary system can be due to the intermolecular S center dot center dot center dot O interaction as the formation -HC=O center dot center dot center dot(O)SO. (C) 2015 Elsevier B.V. All rights reserved.