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The Zn/Sn ratio in Cu2ZnSn(S, Se)4 (CZTSSe) films has been regulated to control the composition-related phase, defect, and photoelectric properties for high performance kesterite solar cells. It is found that the increase in the Zn/Sn ratio can slightly narrow the energy band gap to extend the light absorption range and improve the photocurrent. Optimal Zn/Sn ratio of 1.39 in CZTSSe film is obtained with the least secondary phase, the lowest defect density, and the longest charge recombination lifetime. Up to 10.1％photoelectric conversion efficiency has been achieved by this composition regulation.