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Abstract The electrocatalytic hydrogen evolution reaction (HER) is one of the most studied and promising processes for hydrogen fuel generation. Single-atom catalysts have been shown to exhibit ultra-high HER catalytic activity, but the harsh preparation conditions and the low single-atom loading hinder their practical applications. Furthermore, promoting hydrogen evolution reaction kinetics, especially in alkaline electrolytes, remains as an important challenge. Herein, Pt/C₆₀catalysts with high-loading, high-dispersion single-atomic platinum anchored on C₆₀are achieved through a room-temperature synthetic strategy. Pt/C₆₀-2 exhibits high HER catalytic performance with a low overpotential (η₁₀) of 25 mV at 10 mA cm⁻². Density functional theory calculations reveal that the Pt-C₆₀polymeric structures in Pt/C₆₀-2 favors water adsorption, and the shell-like charge redistribution around the Pt-bonding region induced by the curved surfaces of two adjacent C₆₀facilitates the desorption of hydrogen, thus favoring fast reaction kinetics for hydrogen evolution.