Replacing the high theoretical potential of anodic water decomposition (oxygen evolution reaction) with the low theoretical potential of urea oxidation reaction (UOR) is an urgent need for hydrogen energy storage and conversion. Cobalt nitride nanoflakes, high-performance bifunctional catalysts supported on nickel foam (Co[Formula: see text]N NF/NF), were synthesized by hydrothermal and calcination method. The morphology and composition of the catalyst were studied by XRD, XPS, SEM, TEM, HRTEM and elemental analysis. In order to conduct electrochemical performance and stability, a two-electrode electrolyzer composed of Co[Formula: see text]N NF/NF as both anode and cathode materials is constructed (Co[Formula: see text]N NF/[Formula: see text]N NF/NF). Only a voltage of 1.687[Formula: see text]V is needed to complete 100[Formula: see text][Formula: see text]. It is much lower than the voltage of Pt/[Formula: see text] (1.816[Formula: see text]V), because of which it is believed that this work provides a valuable route for the design of inexpensive and efficient urea electrolysis-assisted hydrogen generation.