A new kind of Ca-based regenerable CO2 absorbent, CaO/Ca12Al14O33, was synthesized on the basis of the integration of CaO, as solid reactant, with a composite metal oxide Ca12Al14O33, as a binder, for applying it to repeated calcination/carbonation cycles. The carbonation reaction can be applied in many industrial processes, and it is important for practical calcination/carbonation processes to have absorbents with high performance. The cyclic carbonation reactivity of the new absorbent was investigated by TGA (thermogravimetric analysis). The effects of the ratio of active material to binder in the new absorbent, the mechanics for preparation, and the reaction process of the high-reactivity CaO/Cal(2)Al(14)O(33) absorbent have been analyzed. The results obtained here indicate that the new absorbent, CaO/Ca12Al14O33, has a significantly improved CO2 absorption capacity and cyclic reaction stability compared with other Ca-based CO2 absorbents. These results suggest that this new absorbent is promising in the application of calcination/carbonation reactions.