Ni–Fe Dual‐Site Polymer Catalyst for High Performance and Stable Electrochemical Urea Synthesis from CO 2 and NO 3 −

The electrochemical synthesis of urea from nitrate (NO 3 − ) and carbon dioxide (CO 2 ) presents a sustainable alternative to conventional methods, mitigating pollution and reducing energy consumption. Herein, a rationally designed Ni–Fe bimetallic pyromellitic acid polymer catalyst (Ni‐PMDA@Fe) is developed for efficient urea electrosynthesis. This metal–organic polymer provides structural robustness, abundant active sites, and a tunable coordination environment, optimizing C–N coupling kinetics. Ni‐PMDA@Fe achieves a urea yield of 449.56 mg h −1 g cat −1 and a Faradaic efficiency (FE) of 41.06% at –0.5 V RHE , significantly surpassing monometallic controls (Ni‐BDC, Ni‐PMDA). Fe incorporation modulates the electronic structure of Ni, enhances charge transfer, and stabilizes key reaction intermediates, enabling synergistic NO 3 − /CO 2 coupling. Comprehensive characterization confirms homogeneous Fe doping and a dual‐metal‐site configuration. Unlike single‐atom or monometallic systems, the Ni–Fe dual‐site architecture optimally tunes the adsorption kinetics of critical intermediates. The catalyst maintains a FE exceeding 30% over a 30 h stability test, demonstrating robust operational stability. Furthermore, techno‐economic analysis (TEA) indicates competitive production costs when powered by renewable energy, highlighting scalability potential. This word demonstrates a practical pathway for sustainable urea synthesis by converting pollutants (NO 3 − /CO 2 ) into value‐added product, thereby contributing to decarbonizing fertilizer production and mitigating nitrogen pollution.