摘要：Electrochemical CO2 reduction is a promising strategy for the utilization of CO2 and intermittent excess *** is the only single metal catalyst that can electrochemically convert CO2 into multicarbon ***,Cu exhibits an unfavorable activity and selectivity for the generation of C2 products because of the insufficient amount of CO*provided for the C‐C *** on the strong CO2 adsorption and ultrafast reaction kinetics of CO*formation on Pd,an intimate CuPd(100)interface was designed to lower the intermediate reaction barriers and improve the efficiency of C2 product *** functional theory(DFT)calculations showed that the CuPd(100)interface enhanced the CO2 adsorption and decreased the CO2*hydrogenation energy barrier,which was beneficial for the C‐C *** potential‐determining step(PDS)barrier of CO2 to C2 products on the CuPd(100)interface was 0.61 eV,which was lower than that on Cu(100)(0.72 eV).Encouraged by the DFT calculation results,the CuPd(100)interface catalyst was prepared by a facile chemical solution method and characterized by transmission electron ***2 temperature‐programmed desorption and gas sensor experiments further confirmed the enhancement of the CO2 adsorption and CO2*hydrogenation ability of the CuPd(100)interface ***,the obtained CuPd(100)interface catalyst exhibited a C2 Faradaic efficiency of 50.3%±1.2%at‒1.4 VRHE in 0.1 M KHCO3,which was 2.1 times higher than that of the Cu catalyst(23.6%±1.5%).This study provides the basis for the rational design of Cu‐based electrocatalysts for the generation of multicarbon products by fine‐tuning the intermediate reaction barriers.