This study describes a unique and sustainable strategy for synthesizing a highly effective photocatalyst using solvothermal synthesis to combine bioderived In2S3 and Nickel Metal-Organic Framework (Ni-MOF) forming In2S3/Ni-MOF. Bioderived In2S3 was produced using Azadirachta indica (neem) leaf extract, providing a green and sustainable source for semiconductor material synthesis. The synergistic interaction of In2S3 with Ni-MOF led to better charge transfer kinetics, a wider band gap, and reduced charge recombination, all contributing to increased photoactivity. The constructed photocatalyst performed admirably under visible light irradiation in producing hydrogen peroxide (H2O2) with an impressive 1528.5 μmol/g.h yield. Furthermore, the photocatalyst demonstrated extraordinary effectiveness in reducing 2,4,6-trinitrophenol (2,4,6-TNP), with a reduction efficiency of 96.31 % in 20 min and high reusability in both applications. The observed results highlight the importance of the collaborative impact between In2S3 and Ni-MOF, demonstrating the promise of this green-synthesized material as a highly efficient photocatalyst with dual uses in various environmental settings. Using renewable neem leaf extract to manufacture In2S3 adds an environmentally beneficial component to the entire strategy, helping to build sustainable and efficient photocatalytic materials.