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Designing atomically dispersed non-precious metal catalysts for 2e− oxygen reduction reaction (ORR) is an appealing strategy to harness O2-to-H2O2 chemistry. Nevertheless, prevailing M–N–C single-atom catalysts (SACs) might still not satisfy the directional regulation of ORR selectivity, hence fail to uphold scalable H2O2 electrosynthesis with a high yield. Herein, we report the precise synthesis of (O,N)-coordinated Fe SAC (FeN2O2) and relating investigation of its performance in H2O2 production over a wide pH range, in comparison with the FeN4 counterpart. Density functional theory simulations reveal that the coordination chemistry engineering has a profound influence on the strength of the oxygen intermediate adsorption. The electron delocalization of M–O configuration readily lowers the d-band center of the Fe metal, which is beneficial to weakening the intermediate adsorption capability and promoting the 2e− ORR process. The thus-derived FeN2O2 exhibits impressive select