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Continuous on-site electrochemical production of hydrogen peroxide (H₂O₂) can provide an attractive alternative to the present anthraquinone-based H₂O₂ production technology. A major challenge in the electrocatalyst design for H₂O₂ production is that O₂ adsorption on the Pt surface thermodynamically favors “side-on” configuration over “end-on” configuration, which leads to a dissociation of O–O bond via dominant 4-electron pathway. This prefers H₂O production rather than H₂O₂ production during the electrochemical oxygen reduction reaction (ORR). In the present work, we demonstrate that controlled coating of Pt catalysts with amorphous carbon layers can induce selective end-on adsorption of O₂ on the Pt surface by eliminating accessible Pt ensemble sites, which allows significantly enhanced H₂O₂ production selectivity in the ORR. Experimental results and theoretical modeling reveal that 4-electron …