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 (Co5.47N 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 Co5.47N NF/NF as both anode and cathode materials is constructed (Co5.47N NF/NF||Co5.47N NF/NF). Only a voltage of 1.687V is needed to complete 100mA⋅cm−2. It is much lower than the voltage of Pt/C||IrO2 (1.816V), 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.