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Experimental and theoretical insights into robust PIL-Br@ZIF-8 hetero-frameworks for the selective conversion of CO 2 into cyclic carbonates under mild conditions. [Display omitted] • A novel strategy is developed for fabricating core–shell PILs@ZIF-8 composites. • PIL-Br@ZIF-8 enables simultaneous adsorption and activation of CO 2 and epoxide. • Low-concentration/low-pressure CO 2 conversion into cyclic carbonates was achieved. • PIL-Br@ZIF-8 is recyclable and exhibits good thermal and structural stability. • Valuable insight into the cycloaddition mechanism is theoretically elucidated. The present study, for the first time, reports the fabrication of core–shell poly(ionic liquids)@ZIF-8 nanocomposites through a facile in-situ polymerization strategy. These composites exhibited exceptional structural characteristics including high specific surface areas and the integration of high-density Lewis acid/base and nucleophilic active sites. The structure–activity relationship, reusability, and versatility of the poly(ionic liquids)@ZIF-8 composites were investigated for the cycloaddition reaction between CO 2 and epoxide. By optimizing the composites structures and their catalytic performance, PIL-Br@ZIF-8(2:1) was identified as an exciting catalyst that exhibits high activity and selectivity in the synthesis of various cyclic carbonates under mild or even atmospheric pressure or simulated flue gas conditions. Moreover, the catalyst demonstrated excellent structural stability while maintaining its catalytic activity throughout multiple usage cycles. By combining DFT calculations, we investigated the transition states and intermediate geometries of the cycloaddition reaction in different coordination microenvironments, thereby proposing a synergistic catalytic mechanism involving multiple active sites. [ABSTRACT FROM AUTHOR]