Carbon dioxide (CO 2 ) fixation into high-valueadded chemicals over eco-friendly heterogeneous catalysts has attracted a long-lasting concern but remains a huge challenge. Herein, we report the efficient metal-/halogen-/solvent-/additivefree heterogeneous CO 2 coupling with aziridines catalyzed by amino acid anion paired mesoporous poly(ionic liquids) (AA-MPILs). A combination of solvothermal synthesis and ion exchange facilely regulated the cations and anions of framework ionic moieties, enabling multifunctional active sites including an acidic carboxyl group, a basic amino group, and a carboxylate as a halogen-free nucleophile with superior leaving ability. The amino group tethered cation and carboxyl groups in the anions promoted the CO 2 adsorption capacity. High yield (>95%) and regioselectivity (>99% for 5-substituted oxazolidinone) and remarkable reusability were reached in the CO 2 cycloaddition with aziridines under mild conditions. The catalyst was also highly active in the coupling of CO 2 with epoxides for the synthesis of cyclic carbonates.

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