Bioinspired Mo‐on‐Cu Nanosheets Enable Potential‐Dependent Electrosynthesis of Urea and Methanol via Interfacial Electron Redistribution

and *NOH coupling accounts for urea formation, while *NO intermediates promote methanol production. This study not only provides a new electrocatalyst for highly efficient urea and methanol electrosynthesis but also can guide the design of other electrocatalysts for high-value chemicals.