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Abstract: A series of porous polymers with different pore volumes, pore sizes, and crosslinking densities were synthesized by high internal phase emulsion (HIPE) polymerization. The crosslinked polymerized HIPEs (polyHIPEs) were formed by the copolymerization of 4-vinylbenzyl chloride and divinylbenzene using water droplets in conventional or Pickering HIPEs as the templates. These porous materials were further modified by quaternization and ion exchange to introduce quaternary ammonium hydroxide groups. The resulting polyHIPEs were utilized as sorbents for reversible CO2 capture from air using the humidity swing. The effect of pore structure on the CO2 adsorption and desorption processes was studied. The polyHIPEs containing large pores and interconnected porous structures showed improved swing sizes and faster adsorption/desorption kinetics of CO2 compared to a commercial Excellion membrane with similar functional groups. [Copyright &y& Elsevier]