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Electric‐driven conversion of carbon dioxide (CO2) to carbon monoxide (CO) under mild reaction conditions offers a promising approach to mitigate the greenhouse effect and the energy crisis. Surface engineering is believed to be one of the prospective methods for enhancing the electrocatalytic activity of CO2 reduction. Herein, hydroxyl (OH) groups were successfully introduced to cadmium nanosheets to form cadmium and cadmium hydroxide nanocomposites (i. e. Cd/Cd(OH)2 nanosheets) via a facile two‐step method. The as‐prepared Cd/Cd(OH)2/CP (CP indicates carbon paper) electrode displays excellent electrocatalytic activity for CO2 reduction to produce CO. The Faradaic efficiency of CO reaches 98.3 % and the current density achieves 23.8 mA cm−2 at −2.0 V vs. Ag/Ag+ in a CO2‐saturated 30 wt% 1‐butyl‐3‐methylimidazole hexafluorophosphate ([Bmim]PF6)‐65 wt% acetonitrile (CH3CN)‐5 wt% water (H2O) electrolyte. And the CO partial current density can reach up to 71.6 mA cm−2 with the CO Faradaic efficiency of more than 85 % at −2.3 V vs. Ag/Ag+, which stands out against Cd/CP, Cd(OH)2/CP, and Cd/CdO/CP electrodes. The excellent electrocatalytic performance of the Cd/Cd(OH)2/CP electrode can be attributed to its unique structural properties, suitable OH groups, perfect interaction with electrolyte, abundant active sites and fast electron transfer rate. [ABSTRACT FROM AUTHOR]