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Abstract Exploring highly efficient hydrogen evolution reaction (HER) electrocatalysts for large‐scale water electrolysis in the full potential of hydrogen (pH) range is highly desirable, but it remains a significant challenge. Herein, a simple pathway is proposed to synthesize a hybrid electrocatalyst by decorating small metallic platinum (Pt) nanosheets on a large nickel telluride nanosheet (termed as Pt Ns /NiTe‐Ns). The as‐prepared Pt Ns /NiTe‐Ns catalyst only requires overpotentials of 72, 162, and 65 mV to reach a high current density of 200 mA cm −2 in alkaline, neutral and acidic conditions, respectively. Theoretical calculations reveal that the combination of metallic Pt and NiTe‐Ns subtly modulates the electronic redistribution at their interface, improves the charge‐transfer kinetics, and enhances the performance of Ni active sites. The synergy between the Pt site and activated Ni site near the interface in Pt Ns /NiTe‐Ns promotes the sluggish water‐dissociation kinetics and optimizes the subsequent oxyhydrogen/hydrogen intermediates (OH*/H*) adsorption, accelerating the HER process. Additionally, the superhydrophilicity and superaerophobicity of Pt Ns /NiTe‐Ns facilitate the mass transfer process and ensure the rapid desorption of generated bubbles, significantly enhancing overall alkaline water/saline water/seawater electrolysis catalytic activity and stability.
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