The CO2 absorption by ionic liquids (ILs) were enhanced by the use of hybrid capsules composed of a core of IL and shell of polyurea and alkylated graphene oxide (GO). These composite structures were synthesized using a Pickering emulsion as a template, and capsules of two different ILs were prepared. The contribution of the encapsulated IL on the CO2 absorption of the capsules is consistent with agitated neat IL, but with an improved mass transfer rate of absorption across different pressures. This novel materials design allows for CO2 to be absorbed significantly faster compared to neat IL and provides insight into improved carbon capture technologies.