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The electronic metal-support interaction (EMSI) of heterogenous catalysts has attracted much attention for its enhancing electrocatalytic efficiency by impacting adsorption and desorption energy of reaction intermediates. Herein, we synthesize the monodispersed single-crystal Pt nanoparticles (~3 nm) decorated on MoS 2 nanosheets with 2 H phase (Pt-MoS 2) by a universal wet chemical method. The morphology and structure characterizations show that the loaded Pt single-crystals are approximately half truncated octahedral shapes enclosed by {1 1 1} and {2 0 0} facets. Benefitting from interfacial electronic structure modulation, the Pt-MoS 2 exhibits a lower overpotential (67.4 mV at the current desity of 10 mA·cm−2), smaller Tafel slope (76.2 mV·dec−1), and robuster HER durability than those of pristine MoS 2 nanosheets and prepared Pt NPs. The theoretical simulations further reveal that the Pt atom at the interface, which belong to {2 0 0} facets and adjoin S atoms, own the smallest hydrogen adsorption free energy by manipulating the d -band center of the Pt metal surface. This work provides crystalline structure and electronic configuration engineering strategy towards to design and develop of metal-support heterostructure with high HER activity and stability. A heterostructure of Pt nanoparticles supported by MoS 2 nanosheets (Pt-MoS 2) is fabricated as a hydrogen evolution reaction (HER) electrocatalyst with high HER activity and stability. The enhanced performance is proved to be ascribed to the interfacial electronic structure modulation. [Display omitted] • HER performance of Pt-MoS 2 heterostructure is significantly enhanced. • Atomic-level structure characterization of Pt-MoS 2 is investigated. • The enhanced catalysis activity is attributed to the interfacial electronic structure modulation. [ABSTRACT FROM AUTHOR]