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Rational design of efficient methanol oxidation reaction (MOR) catalyst that undergo non‐CO pathway is essential to resolve the long‐standing poisoning issue. However, it remains a huge challenge due to the rather difficulty in maximizing the non‐CO pathway by the selective coupling between the key *CHO and *OH intermediates. Here, we report a high‐performance electrocatalyst of patchy atomic‐layer Pt epitaxial growth on CeO2 nanocube (Pt ALs/CeO2) with maximum electronic metal‐support interaction for enhancing the coupling selectively. The small‐size monolayer material achieves an optimal geometrical distance between edge Pt−O−Ce sites and *OH absorbed on CeO2, which well restrains the dehydrogenation of *CHO, resulting in the non‐CO pathway. Meanwhile, the *CHO/*CO intermediate generated at inner Pt−O−Ce sites can migrate to edge, inducing the subsequent coupling reaction, thus avoiding poisoning while promoting reaction efficiency. Consequently, Pt ALs/CeO2 exhibits exceptionally catalytic stability with negligible degradation even under 1000 s pure CO poisoning operation and high mass activity (14.87 A/mgPt), enabling it one of the best‐performing alkali‐stable MOR catalysts. [ABSTRACT FROM AUTHOR]

Knowledge of the photocatalytic H2 evolution mechanism is of great importance for designing active catalysts toward a sustainable energy supply. An atomic-level insight, design, and fabrication of single-site Co1-N4 composite as a prototypical photocatalyst for efficient H2 production is reported. Correlated atomic characterizations verify that atomically dispersed Co atoms are successfully grafted by covalently forming a Co1-N4 structure on g-C3N4 nanosheets by atomic layer deposition. Different from the conventional homolytic or heterolytic pathway, theoretical investigations reveal that the coordinated donor nitrogen increases the electron density and lowers the formation barrier of key Co hydride intermediate, thereby accelerating H-H coupling to facilitate H2 generation. As a result, the composite photocatalyst exhibits a robust H2 production activity up to 10.8 μmol h−1, 11 times higher than that of pristine counterpart. [ABSTRACT FROM AUTHOR]