The reaction of m-xylylenediamine (mXD) with carbon dioxide was examined and its feasibility as a sequestration material of carbon dioxide was discussed. The reaction was monitored by using the FT-IR and gravitational methods, while the crystalline structure of the reaction product was investigated with elemental analysis, powder Xray diffraction, single crystallography, and 13C MAS NMR spectroscopy. Even at ambient temperature, mXD reacted with carbon dioxide of low partial pressure in the atmosphere and produced a 1 : 1 molar adduct which appeared as a white crystalline material. The hydrogen bonds that formed between the adduct molecules resulted in the formation of a stable crystal. The sequestration capacity of mXD was very great, ~280mg gmXD ^(-1) below 50 ℃. An adsorbent prepared by dispersing mXD on silica was capable of capturing carbon dioxide, but it could be regenerated by evacuating at 25 ℃.