To address the challenges of high carrier recombination rate, narrow light response range and instability of the metal sulfides photocatalyst, ZnIn2S4 nanosheet is modified by Ni-S bonds and S vacancies (SV) through a solvothermal and light assisted impregnation methods. It should be noted that the S of Ni-S bonds is offered by the ZnIn2S4 nanosheet. In addition, the SV are generated on the surface of the ZnIn2S4 nanosheet through the induction of Ni-S bonds. Furthermore, compared with the initial ZnIn2S4 nanosheet, the modified ZnIn2S4 nanosheet exhibits more superior property of photocatalytic H2 production. Under visible light or simulated sunlight irradiation, the H2 production rate of the modified ZnIn2S4 nanosheet is 1486 and 6071 μmol·g-1·h-1, and it is almost 3.9 and 4.4 times higher than that of the initial ZnIn2S4 nanosheet. In addition, combined with the analyses of microstructure characterizations, photoelectric properties, theoretical calculations and in situ XPS, the superior property of the modified ZnIn2S4 nanosheet is attributed to the synergistic effects of the Ni-S bonds and SV. Because the Ni-S bonds and SV can significantly enhance the separation efficiency of the photoproduced electron-holes and offer abundant active sites for H2 production. This study offers an innovative perspective for optimizing the metal sulfides to improve their photocatalytic H2 evolution property.