Electrocatalytic/photocatalytic　C─N　coupling　from　small　carboncontaining　(such　as　CO2　and　CH3OH)　and　nitrogen-containing　species　(such　as　N2,　NO3−,　and　NH3)　enables　the　synthesis　of　value-added　organonitrogen　compounds,　including　urea,　amides,　and　amino　acids.　This　approach,　ideally　driven　by　renewable　energy,　holds　great　promise　for　sustainable　developments　and　has　thus　been　attracting　increasing　research　interest　in　recent　years.　To　enhance　the　C─N　coupling　under　mild　reaction　conditions,　it　is　necessary　to　activate　different　substrate　molecules　effectively　and　balance　the　adsorption　and　desorption　of　various　C-　and　N-containing　intermediates　and/or　radicals,　thereby　realizing　different　value-added　organonitrogen　compounds.　In　this　review,　the　recent　advances　in　electrocatalytic/photocatalytic　C─N　coupling　reactions　targeting　those　three　types　of　products,　i.e.,　urea,　amides,　and　amino　acids　is　aimed　to　summarized.　The　rational　designs　of　active　sites　for　synergistic　catalysis　are　discussed,　including　their　types,　compositions,　spatial　arrangements,　crystal　facets,　heterostructures,　and　local　environments.　Different　reactant　molecules　and　catalytic　mechanisms　for　the　electrocatalytic/photocatalytic　C─N　coupling　reactions,　as　well　as　the　methods　of　C─N　coupling　products　detection,　are　also　described.　Finally,　the　existing　challenges　in　this　field　are　summarized,　and　the　potential　research　perspectives　are　also　proposed.　©　2025　Wiley-VCH　GmbH.