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We demonstrate that wafer-scale, transferable, and transparent thin-film catalysts based on MoS2, which consists of cheap and earth abundant elements, can provide a low onset potential of 1 mA cm−2 at 0.17 V versus a reversible hydrogen electrode and the high photocurrent density of 24.6 mA cm−2 at 0 V for a p-type Si photocathode. c-Domains with vertically stacked (100) planes in the transferable 2H-MoS2 thin films, which are grown via a thermolysis method, act as active sites for the hydrogen evolution reaction, and photogenerated electrons are efficiently transported through the n-MoS2/p-Si heterojunction.