Multidimensional Engineering Enabling Rate‐Matched C−N Coupling for Efficient Organonitrogen Electrosynthesis

Electrochemical C−N coupling has emerged as a promising alternative to energy‐intensive synthetic routes for sustainable organonitrogen synthesis (e.g., urea, amides, amines, amino acids, oximes, and nitriles). By utilizing diverse carbon and nitrogen feedstocks, such as CO 2 and nitrogen oxides (NO x ), this approach advances carbon/nitrogen neutrality and simultaneously produces value‐added products. However, practical implementation remains challenging because of sluggish reactant adsorption, complex reaction networks, competing side reactions, and kinetic mismatches between carbon‐ and nitrogen‐containing intermediates. In this review, we validate rate matching as a critical design concept governing efficient C−N coupling and systematically summarize recent advances in the electrosynthesis of organonitrogen chemicals. We first review critical adsorbed intermediates and in‐depth C−N coupling pathways. Multidimensional engineering strategies are then categorized into catalyst‐, interface‐, and reactor‐level management and discussed, corresponding respectively to electrocatalyst design, electrolyte microenvironment modulation, and electrolyzer architecture. Furthermore, we elaborate on how the distinct functions of these strategies contribute to synchronizing C−N coupling. Finally, we conclude with remaining challenges and future perspectives toward efficient and scalable electrocatalytic synthesis of organonitrogen molecules.