In previous research, we have found and reported for the first time that β-alanine aqueous solution could be employed to efficiently separate SO 2 from flue gas. However, the performance of most natural amino acids (AAs) on SO 2 absorption and their interaction mechanisms are not fully understood. In this work, the performance of 20 natural AA aqueous solutions on SO 2 absorption from flue gas was systematically studied. The experimental data showed that monoamino AAs (MAAs) exhibited good absorption performance, especially glycine, of which the saturation uptake of SO 2 reached 0.461 g/g. All the MAAs showed excellent regeneration performance, while the polyamino AAs of lysine, arginine, and histidine performed poorly. Based on the characterization and analysis using Fourier transform infrared spectroscopy, Raman spectroscopy, 13 C-nuclear magnetic resonance, and the density-functional theory simulation, it was found that the interaction mechanism between MAA aqueous solutions represented by glycine and SO 2 is complex, including the hydrolysis of SO 2 and the protonation of MAAs, the formation of hydrogen bonds between cationic MAAs and HSO 3 − , and the interaction between zwitterionic MAAs and SO 2 . In addition, cationic glycine could form a carboxylic acid dimer, which further interacted with HSO 3 − through hydrogen bonds.