Photocatalytic hydrogen (H-2) generation through water splitting has attracted substantial attention as a clean and renewable energy generation process that has enormous potential in converting solar-to-chemical energy using suitable photocatalysts. The major bottleneck in the development of semiconductor-based photocatalysts lies in poor light absorption and fast recombination of photogenerated electron-hole pairs. Herein we report the synthesis of CuS/TiO2 heterostructured nanocomposites with varied TiO2 contents via simple hydrothermal and solution-based process. The morphology, crystal structure, composition, and optical properties of the as-synthesized CuS/TiO2 hybrids are evaluated in detail. Controlling the CuS/TiO2 ratio to an optimum value leads to the highest photocatalytic H-2 production rate of 1262 mu mol h(-1) g(-1), which is 9.7 and 9.3 times higher than that of pristine TiO2 nanospindles and CuS nanoflakes under irradiation, respectively. The enhancement in the H-2 evolution rate is attributed to increased light absorption and efficient charge separation with an optimum CuS coverage on TiO2. The photoluminescence and photoelectrochemical measurements further confirm the efficient separation of charge carriers in the CuS/TiO2 hybrid. The mechanism and synergistic role of CuS and TiO2 semiconductors for enhanced photoactivity is further delineated.