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Three ionic liquid (IL) monomers consisting of one, two, and four benzene rings were designed with 2-phenylimidazole and polymerized with α,α′-dichloro-p-xylene (DCX) and formaldehyde dimethyl acetal (FDA) to form a series of novel poly(ionic liquid)s (PILs). In this process, the designed ILs were employed as active ionic sites, and DCX and FDA were selected as cross-linkers. Self-condensation of the cross-linker provided a large specific surface area for the hypercross-linked organic framework, while cocondensation between the cross-linker and IL introduced active sites to the framework. The obtained porous hypercross-linked PILs not only promoted CO 2 capture and the selective absorption of CO 2 /N 2 but also showed good activity for the cycloaddition of epoxide with CO 2 . HP-[BZPhIm]Cl-DCX-1 with a large surface area (763 m 2 •g −1 ) showed a CO 2 uptake capacity of 1.47 mmol•g −1 and offered a 98.9% yield of the CO 2 cycloaddition product with epichlorohydrin at 80 °C for 24 h under 0.1 MPa CO 2 pressure. The designed PILs provide an important reaction for CO 2 utilization.