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This article presents a comprehensive study of CO2 capture using a new composite of Montmorillonite and Choline-Chloride-Urea in a continous fixed-bed adsorption system. The results revealed superior performance of a surface-activated mesoporous support compared to the unmodified solid support. The breakthrough curves, adsorption capacities, regenerability, and CO2/N2 selectivity of the developed nano-caly adsorbent were also studied for the first time. The ANOVA analysis indicated highly significant effects of gas flow rate and CO2 vol. % on breakthrough-time and adsorption capacity. The kinetic mathematical models were applied for breakthrough curve analysis. Clark model fitted to the experimental data better than others.