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Abstract Copper (Cu) is the most attractive electrocatalyst for CO₂reduction to multi‐carbon (C₂₊) products with high economic value in considerable amounts. However, the rational design of a structurally stable Cu‐based catalyst that can achieve high activity and stability towards C₂₊products remain a grand challenge. Here, a highly stable nickel oxygenate/Cu electrocatalyst is developed with abundant NiOOH/Cu interfaces by in situ electrochemical reconstruction. The nickel oxygenate/Cu electrocatalyst achieves a superior Faradaic efficiency of 86.3 ± 3.0% and a record partial current density of 2085 A g⁻¹for C₂₊products with long‐term stability. In situ experimental and theoretical studies demonstrates that the exceptional performance in generating C₂₊products is attributed to the presence of the NiOOH/Cu interfaces which increase *CO coverage, lower energy barrier for *CO coupling and stabilize *OCCO simultaneously. This work provides new insights into the rational design of electrocatalysts to achieve stable and efficient electrocatalytic CO₂reduction capabilities.