Calcium looping (CaL) integrated with methane dry reforming (DRM) shows promise for carbon capture and utilization. To enhance the CaL− DRM tandem processes, a raspberry-structured aerosol dual-functional material composed of CaO (CO 2 adsorbent), Ni (DRM catalyst), and CeO 2 (promoter) was fabricated via gas-phase evaporation-induced self-assembly. The utilization of Ca−Ni−Ce is highly beneficial by the creation of metal−support−promoter interaction for promoting an effective carbon capture followed by interfacial catalysis, providing an alternative pathway with enhanced redox ability and reduction of activation energy. The Ca−Ni−Ce composite materials with clustered particle characteristics showed great improvement in the performance of cyclic CaL−DRM in comparison to the reported values: low required carbonation/decarbonation temperatures (400/600 °C), high CO 2 uptake efficiency (12.1 mmol COd 2 /g CaO ), ultrahigh CO 2 conversion (97.2%) under relatively low-temperature operation (600 °C), and sufficiently high operational stability. Overall, the proposed Ca−Ni−Ce hybrid material fabricated via the aerosol synthetic method demonstrates significant advances in the low-temperature CaL−DRM processes, showing promise as a sustainable chemical engineering route for industrial applications.