Developing　novel　electrocatalysts　for　achieving　high　selectivity　and　faradaic　efficiency　in　the　carbon　dioxide　reduction　reaction　(CO2RR)　poses　a　major　challenge.　In　this　study,　a　catalyst　featuring　a　nitrogen-doped　carbon　shell-coated　Ni　nanoparticle　structure　is　designed　for　efficient　carbon　dioxide　(CO2)　electroreduction　to　carbon　monoxide　(CO).　The　optimal　Ni@NC-1000　catalyst　exhibits　remarkable　CO　faradaic　efficiency　(FECO)　values　exceeding　90%　across　a　broad　potential　range　of　−0.55　to　−0.9　V　(vs.　RHE),　and　attains　the　maximum　FECO　of　95.6%　at　−0.75　V　(vs.　RHE)　in　0.5　M　NaHCO3.　This　catalyst　exhibits　sustained　carbon　dioxide　electroreduction　activity　with　negligible　decay　after　continuous　electrolysis　for　20　h.　More　encouragingly,　a　substantial　current　density　of　200.3　mA　cm−2　is　achieved　in　a　flow　cell　at　−0.9　V　(vs.　RHE),　reaching　an　industrial-level　current　density.　In　situ　Fourier　transform　infrared　spectroscopy　and　theoretical　calculations　demonstrate　that　its　excellent　catalytic　performance　is　attributed　to　highly　active　pyrrolic　nitrogen　sites,　promoting　CO2　activation　and　significantly　reducing　the　energy　barrier　for　generating　*COOH.　To　a　considerable　extent,　this　work　presents　an　effective　strategy　for　developing　high-efficiency　catalysts　for　electrochemical　CO2　reduction　across　a　wide　potential　window.　©　2024　The　Royal　Society　of　Chemistry.