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Abstract In this work, a new type of multifunctional materials (MFMs) called self‐regenerative Ni‐doped CaTiO₃/CaO is introduced for the integrated CO₂capture and dry reforming of methane (ICCDRM). These materials consist of a catalytically active Ni‐doped CaTiO₃and a CO₂sorbent, CaO. The article proposes a concept where the Ni catalyst can be regenerated in situ, which is crucial for ICCDRM. Exsolved Ni nanoparticles are evenly distributed on the surface of CaTiO₃under H₂or CH₄, and are re‐dispersed back into the CaTiO₃lattice under CO₂. The Ni‐doped CaTiO₃/CaO MFMs show stable CO₂capture capacity and syngas productivity for 30 cycles of ICCDRM. The presence of CaTiO₃between CaO grains prevents CaO/CaCO₃thermal sintering during carbonation and decarbonation. Moreover, the strong interaction of CaTiO₃with exsolved Ni mitigates severe accumulation of coke deposition. This concept can be useful for developing MFMs with improved properties that can advance integrated carbon capture and conversion.