The global shift toward sustainable energy requires the development of efficient hydrogen production. In this work, zinc oxysulfide (ZnOS) photocatalysts were produced by the hydrothermal method, where careful control of precursor ratios, reaction temperatures, and annealing conditions enabled a precise tuning of structural and optical properties. Experimental characterization also demonstrated that annealing transforms initially rough, spherical ZnOS particles into smoother, highly crystalline forms, as evidenced in scanning electron microscope (SEM) and X-ray diffraction (XRD). Ultra-violet visible (UV–Vis) absorption spectroscopy reveals significant enhancements in visible light absorption within the 350 nm range, indicating changes in electronic structures and increased charge separation. Ultimately, the successful deposition of ZnOS films onto glass substrates demonstrates the scalability and adaptability of our synthesis route for optoelectronic applications. This work offers new insights into the behavior of synthesis parameters and photocatalytic performance, suggesting a promising path forward for the preparation of high-performance, tunable ZnOS materials for sustainable hydrogen production.