The conventional industrial production of nitrogen‐containing fertilizers, such as urea and ammonia, relies heavily on energy‐intensive processes, accounting for approximately 3 % of global annual CO2 emissions. Herein, we report a sustainable electrocatalytic approach that realizes direct and selective synthesis of urea and ammonia from co‐reduction of CO2 and nitrates under ambient conditions. With the assistance of a copper (Cu)‐based salphen organic catalyst, outstanding urea (3.64 mg h−1 mgcat−1) and ammonia (9.73 mg h−1 mgcat−1) yield rates are achieved, in addition to a remarkable Faradaic efficiency of 57.9±3 % for the former. This work proposes an appealing sustainable route to converting greenhouse gas and waste nitrates by renewable energies into value‐added fertilizers.

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Despite of superior performance of the oxide-derived copper (OD-Cu) in producing valuable hydrocarbons during CORR, its fabrication process is still ambiguous and complicated. In this work, we develop a simple microwave-assisted method to synthesize the oxide-derived Cu nanosheet (OD-Cu NS) and reveal that the oxidation state of Cu species is controlled by varying the Cu precursor amount. Notably, the simultaneous formation of nano-sized Cu domains influence the surface roughness of OD-Cu NS. The partially oxidized Cu surface exhibits a superior faradaic efficiency (FE) of C products up to 72%, along with a partial current density of 55 mA cm in a neutral KHCO solution. More importantly, the as-obtained OD-Cu NS shows a synergetic effect on dissociating of CO molecules by the strong binding energy and promoting of C compounds productivity by the enlarged electrochemical surface area. This work provides a new insight for designing efficient OD-Cu catalysts towards CORR.