In the realm of photocatalysis, the creation of clean and pollution-free composite material catalysts is critical. Electrostatic self-assembly techniques were used in this study to construct ZnIn2S4 nanosheets onto the surface of Cu-MOF, culminating in the development of a unique Cu-MOF/ZnIn2S4 composite catalyst. Cu-MOF was shown to have a strong interface impact with ZnIn2S4, which resulted in a large increase in the number of active sites and, consequently, the efficiency of hydrogen generation. This was demonstrated by a number of parameters. The Cu-MOF/ZnIn2S4-10 composite material's optimum hydrogen evolution rate was 0.3 mmol h−1g−1, which was 2.14 times larger than that of pure ZnIn2S4 nanosheets (0.14 mmol h−1g−1). Furthermore, the development of Cu-MOF/ZnIn2S4 heterojunctions considerably improved ZnIn2S4's deficiencies in photocatalytic hydrogen production, increasing charge separation rates and providing a viable approach to improve ZnIn2S4's hydrogen production efficiency.