Electrochemical　CO2　reduction　reaction　(CO2RR)　provides　a　promising　route　to　converting　CO2　into　value-added　chemicals　and　to　neutralizing　the　greenhouse　gas　emission.　For　the　industrial　application　of　CO2RR,　high-performance　electrocatalysts　featuring　high　activities　and　selectivities　are　essential.　It　has　been　demonstrated　that　customizing　the　catalyst　surface/interface　structures　allows　for　high-precision　control　over　the　microenvironment　for　catalysis　as　well　as　the　adsorption/desorption　behaviors　of　key　reaction　intermediates　in　CO2RR,　thereby　elevating　the　activity,　selectivity　and　stability　of　the　electrocatalysts.　In　this　paper,　we　review　the　progress　in　customizing　the　surface/interface　structures　for　CO2RR　electrocatalysts　(including　atomic-site　catalysts,　metal　catalysts,　and　metal/oxide　catalysts).　From　the　perspectives　of　coordination　engineering,　atomic　interface　design,　surface　modification,　and　hetero-interface　construction,　we　delineate　the　resulting　specific　alterations　in　surface/interface　structures,　and　their　effect　on　the　CO2RR　process.　At　the　end　of　this　review,　we　present　a　brief　discussion　and　outlook　on　the　current　challenges　and　future　directions　for　achieving　high-efficiency　CO2RR　via　surface/interface　engineering.　©　2024　The　Royal　Society　of　Chemistry.