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Inspired by the unique band structure of CsPbBr3, we have developed an asymmetric Cl‐exchange strategy based on the CsPbBrxCl3‐x/TiO2 heterojunction‐type catalyst and achieved photocatalytic activation of C(sp3)−H bond using the toluene oxidation reaction as a proof‐of‐concept application. The anion exchange at the supported CsPbBr3 surface results in the CsPbBrxCl3‐x/TiO2 structure with an asymmetric distribution of halide. The resultant heterojunction‐type catalysts exhibit significantly improved photocatalytic activity for toluene oxidation reaction with the highest benzaldehyde production rate at 1874 μmol g−1 h−1 (∼4 times that of the naked CsPbBr3 nanocrystals). The remarkable photocatalytic performance can be ascribed to the improved carrier transport at CsPbBrxCl3‐x/TiO2 interface enabled by the unique band structure due to the asymmetric halide distribution, verified by the micro‐strain discovered through the X‐ray diffraction. This work demonstrates a new pathway to fabricate highly‐efficient halide perovskite heterojunction‐type catalysts for photocatalytic activation of C(sp3)−H bond. [ABSTRACT FROM AUTHOR]