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The calcium-barium (Ca–Ba) composite adsorbents based on CO2 storage material (CO2SM, the white solid material formed by the absorption of carbon dioxide in a binary hybrid system of tetraethylene glycol and 1,3-propylene diamine) for CO2 adsorption were systematically investigated, including the synthesis conditions of adsorbent precursors and adsorption conditions. The experimental results showed that the maximum adsorption capacity of the Ca–Ba-5 adsorbent for CO2 was 621 mg g−1 under the conditions of 15g L−1 CO2SM, molar ratio of Ca:Ba 9:1, hydrothermal reaction temperature 100℃ and hydrothermal reaction time 90 min. Moreover, the evaluation of the adsorption performance of the samples for 15 consecutive cycles suggested that the Ca–Ba-5 adsorbent exhibited relatively stable adsorption performance and its adsorption performance stability was improved by 18% than that of CaO adsorbent prepared under the same conditions. Moreover, the cyclic performance of the Ca–Ba-5 adsorbent from the 2nd to the 15th cycle was the most stable and only decreased 10%. [ABSTRACT FROM AUTHOR]