Replacing dynamics-restricted oxygen evolution reaction (OER) with smart urea oxidation reaction (UOR) is very important for reducing the power consumption for hydrogen production. Here, the Co3Mo3N-400/NF is prepared using a facial way, which exhibits remarkable catalytic performances for UOR, hydrogen evolution reaction (HER) and overall urea electrolysis (OUE) because of the more exposed active sites and high electrical conductivity. At 100 mA/cm2, the Co3Mo3N-400/NF shows a small potential of 1.356 V vs. RHE (reversible hydrogen electrode) for UOR, which is much lower than that for OER. Furthermore, for HER, to reach to 100 mA/cm2, a low overpotential of 299 mV is required, and the urea has negligible influence on the HER process. For OUE, the Co3Mo3N-400/NF||Co3Mo3N-400/NF shows a small cell potential of 1.481 V at 100 mA/cm2 along with a good durability. Our work provides more choice for future OUE to generate hydrogen.