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Development of effective non-noble electrocatalysts for hydrogen evolution reaction (HER) is crucial for hydrogen production by water electrolysis. Herein, several composite catalysts of non-stoichiometric Mo6S9.5 films grown on graphene-like N-doped carbon films were prepared and evaluated for HER in 0.5 M H2SO4. The unique structure endowed the catalysts with highly exposed edge active sites, high specific surface area and prominently high activities for HER. The optimized catalyst exhibited a low overpotential of 113 mV at 10 mA/cm2, a low Tafel slope of 64 mV/dec, and a low charge transfer resistance of 40 Ω along with a highly catalytic stability.