The electrochemical coupling of biomass oxidation and nitrogen conversion presents a potential strategy for high value‐added chemicals and nitrogen cycling. Herein, in this work, CuO/Co3O4 with heterogeneous interface is successfully constructed as a bifunctional catalyst for the electrooxidation of 5‐hydroxymethylfurfural to 2,5‐furandicarboxylic acid and the electroreduction of nitrate to ammonia (NH3). The open‐circuit potential spontaneous experiment shows that more 5‐hydroxymethylfurfural molecules are adsorbed in the Helmholtz layer of the CuO/Co3O4 composite, which certifies that the CuO/Co3O4 heterostructure is conducive to the kinetic adsorption of 5‐hydroxymethylfurfural. In situ electrochemical impedance spectroscopy further shows that CuO/Co3O4 has faster reaction kinetics and lower reaction potential in oxygen evolution reaction and 5‐hydroxymethylfurfural electrocatalytic oxidation. Moreover, CuO/Co3O4 also has a good reduction effect on . The ex‐situ Raman spectroscopy shows that under the reduction potential, the metal oxide is reduced, and the generated Cu2O can be used as a new active site for the reaction to promote the electrocatalytic conversion of to NH3 synthesis. This work provides valuable guidance for the synthesis of value‐added chemicals by 5‐hydroxymethylfurfural electrocatalytic oxidation coupled with while efficiently producing NH3.