Electrochemical reduction of CO 2 comprising the CO 2 reduction reactuib (CO 2 RR) and oxygen evolution reaction (OER) is one of the most promising technologies for electrification of the chemical process industry. Here, the performance of a electrocatalyst with a three-dimensional structure of InZnCu on Cu foam (CF) is presented. This electrocatalyst was fabricated by electrodeposition of In and Zn over Cu and exhibited a superior reduction of CO 2 to CO at a Faradaic efficiency of 93.7% at −0.7 V and an excellently long duration of 100 h. Due to the synergy of the thin In layer, the Zn nanosheets provided a high surface-active area and strong mechanical robustness during the reaction. Additionally, a two-electrode system was constructed based on the CF-modified surface, which provided valuable guidelines on the overall CO 2 RR−OER system for further evolution. Furthermore, due to the facile synthesis, the bimetal-layer double hydroxide (LDH) exhibited high conductivity and high OER performance. Hence, the two-electrode system assembled excellent electrocatalysts for the CO 2 RR−OER (InZnCu/CF||Cu(OH) 2 NWs@NiCo-LDH/CF) with high conversions of CO 2 to CO of 67% and 88% at 2 and 50 mA cm −2 , respectively. Notably, the CO 2 RR−OER system exhibited excellent stability in a 40 h CO 2 conversion with a constant current density of 2 mA cm −2 at an ultralow voltage of 1.59 V. Moreover, the calculation of the energy input converting CO per ton of CO 2 resulted in a low energy input range for further development in scalability. This overall CO 2 RR−OER proposes development in electrochemical CO 2 reduction for industrial applications.