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Cu‐based catalysts exhibit excellent performance in hydrogenation reactions. However, the poor stability of Cu catalysts under high temperatures has restricted their practical applications. The preparation of stable Cu catalysts supported by SiO2 with strong metal–support interaction (SMSI) has thus aroused great interest due to the high abundance, low toxicity, feasible processability, and low cost of SiO2. The challenge in the construction of such SMSI remains to be the inertness of SiO2. Herein, a simple and scalable method is developed to prepare 2D silica (2DSiO2) supported Cu catalysts with SMSI by carefully manipulating the topological exfoliation of CaSi2 with CuCl2 and thereafter calcination. The prepared Cu‐2DSiO2 catalysts with the unique encapsulated Cu nanoparticles exhibit excellent activity and long‐term stability in high‐temperature CO2 hydrogenation reactions. This feasible and low‐cost solution for stabilizing Cu catalysts might shed light on their realistic applications. [ABSTRACT FROM AUTHOR]