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Photocatalysis is an effective means to convert CO2 and solar energy into high value-added chemicals. Herein, the surface gradient S doped CuCo2O4 microflowers were fabricated by an in situ topotactic engineering strategy. This photocatalyst presented CO2 photoreduction with a satisfying activity (5 h, 181 μmol) and stability (94.5% retention). Additionally, the theoretical calculations indicated the fomated M-S bond could be favorbale to facilitate the initial CO2⁎ binding and promote the formation of COOH⁎ intermediates. This work provides a novel strategy for the fabrication of effective photocatalysts and highlights an in-depth understanding of micro-level regulation towards photocatalytic overall performance.