Ionic liquids (ILs) as the solvents for carbon dioxide (CO2), with high capacity and selectivity, are promising candidates for CO2 capture. Developing methods such as microencapsulation that enable the cost-effective and regenerable operation using ILs-based absorbent is of paramount importance to carbon capture and management technologies. In this study, we investigated the feasibility of IL encapsulation within a polymeric shell and evaluated the performance of the capsules in CO2 absorption from the gas phase. We learned that encapsulation enhances the intrinsic capacity of an ionic liquid in CO2 sorption. The proper choice of chemistry for the polymeric matrix and the high specific surface area of the capsules allows the encapsulated ILs to outperform their liquid counterpart. We report unprecedented recyclability, encapsulation retention, and absorption capacity for the encapsulated IL absorbent designed for CO2 sorption. We observed a synergistic effect on the CO2 absorption capacity of the capsules as a result of using a fluorine-containing polymer.