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Carbon dioxide electroreduction driven by renewable electricity into high‐value chemicals enables energy storage while contributing to climate change mitigation. Herein, a CuPd bimetallic catalyst is developed by electrodeposition for efficient CO2 electroreduction, achieving a C2+ Faradaic efficiency as high as 75.6% with a current density of −200 mA cm−2 at −1.15 V versus reversible hydrogen electrode. Upon incorporation of Pd, the average d‐band center of the CuPd bimetallic catalyst downward shifts relative to the Fermi level, making the adsorbed CO intermediates active for further C–C coupling. Theoretical calculations confirm that CO generated on the Pd domain can spill over to the CuPd interface for C–C coupling with a lower energy barrier, further promoting the formation of C2+ compounds. This study provides insights into the rational design of Cu‐based bimetallic catalysts for highly efficient CO2 electroreduction to multicarbon products.