A new adsorbent based on sterically hindered amine for efficient CO2 capture was prepared. Mesoporous silicon MCM-41 was modified by sterically hindered amine AMPD (2-amino-2-methyl-1,3-propanediol) in different AMPD loadings by a facile solid-state self-assembly approach. The physicochemical properties of the MCM-41@AMPD composites were analyzed using XRD, BET, FT-IR and SEM, and the composites were investigated for the CO2 capture performance, including CO2 capture capacity, adsorption selectivity and cycling stability. Characterization analyses showed that the AMPD active components were successfully incorporated and well dispersed into the mesoporous silicon MCM-41 surfaces. Adsorption results suggest that the modification by the active ingredient AMPD can significantly improve the CO2 capture performance. The MCM-41@AMPD material with an AMPD loading of 7mmol∙g-1 MCM-41 support exhibits a good CO2 adsorption capacity and CO2 adsorption selectivity, and shows excellent cycling stability. Furthermore, the isosteric heat of CO2 adsorption on the MCM-41@AMPD-7 material was evaluated by the Clausius-Clapeyron equation, and the value was 34-78 kJ∙mol-01.