Constructing Enzyme‐Inspired Multisite Synergistic Catalyst for Promoting CO ₂ Electroreduction to Ethylene at pH Universal Condition

ABSTRACT Natural enzymes achieve high catalytic efficiency through the cooperative integration of catalytic centers, substrate‐binding sites, and a regulated local water environment. Inspired by this principle, we report an enzyme‐functional electrocatalyst that integrates these key elements into a Cu‐based architecture through molecular amine modification. The resulting multisite catalyst enables highly selective electrochemical CO ₂ reduction to ethylene (C ₂ H ₄ ) with Faradaic efficiencies among the highest reported under pH‐universal conditions, delivering values of 64.5%, 72.0%, and 74.6% in acidic, neutral, and alkaline electrolytes, respectively. Mechanistic studies reveal that amine modification not only enhances CO ₂ binding and *CO stabilization on Cu but also tailors the interfacial water structure by constructing a hydrogen‐bond network and suppressing excessive free water, thereby optimizing proton transfer and *CO/*H competition. This work establishes enzyme‐inspired interfacial water regulation as an effective strategy for selective CO ₂ ‐to‐C ₂ H ₄ conversion.