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Features of thermochemical treatment of nanostructured tungsten trioxide (WO3) films in hydrogen sulfide aimed at the formation of tungsten disulfide (WS2) nanolayers in the hybrid WS2/WO3 structure are investigated. The effect of temperature and treatment time on the structure, chemical state, morphology, and optical properties of the WS2/WO3/FTO photocathode (on the fluorinated tin oxide substrate), as well as on its photoelectrocatalytic activity in the reaction of hydrogen evolution in an acidic solution has been established. It is shown that sulfurization of nano-needle WO3 films under optimal conditions leads to the formation of a nanocrystalline hybrid WS2/WO3 structure that ensures the separation of photogenerated carriers (electrons and holes) at interphase boundaries (heterojunctions). This facilitates the efficient photo-activated hydrogen evolution reaction according to the Z-scheme. First-principal calculations of the thermodynamic properties of the hybrid WS2/WO3 nanocatalyst showed that a synergistic effect of nanophases is possible. This increases the catalytic activity of hydrogen evolution on both the basal planes of WS2 nanoclusters and the surface of metal oxide nanoclusters.