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MoS₂ composed of earth‐abundant elements is considered as a promising hydrogen evolution reaction (HER) catalyst for p‐type Si photocathode owing to its appropriate hydrogen adsorption free energy for the edge sites and high photochemical stability in acidic electrolytes. However, the direct synthesis of uniform and atomically thin MoS₂ on Si by usual chemical vapor deposition techniques remains challenging because of the weak van der Waals interaction between Si and MoS₂. Herein, by controlling the gas phase kinetics during metal–organic chemical vapor deposition, wafer‐scale direct synthesis of 3D MoS₂ films on TiO₂‐coated p‐type Si substrates is demonstrated. The 3D MoS₂ layer with a number of edge sites exposed to ambient substantially reduces the HER overpotential of Si photocathode and simultaneously increases the saturation current density due to the antireflection effect. Directly grown …