Urea electrolysis offers a promising approach for converting urea-rich wastewater into hydrogen, contributing to environmental preservation and sustainable energy production. The electrocatalytic urea oxidation reaction (UOR) holds great potential in replacing the oxygen evolution reaction (OER) for enhancing cathodic hydrogen evolution due to its lower equilibrium potential. However, conventional urea electrolysis processes suffer from drawbacks such as high energy consumption, high overpotential, and poor stability, necessitating the development of high-performance catalysts. In this study, a superior NiCo-LDHs/VMT catalyst prepared via a hydrothermal method exhibited efficient urea electrolysis, producing nitrogen gas under a current density of 10 mA·cm-2 and a potential of 1.35 V, as well as hydrogen gas under a potential of -0.225 V. These results demonstrate the potential of this method for industrial-scale urea electrolysis, providing insights for the high-value utilization of zeolite resources in Xinjiang and the efficient design of urea electrolysis catalysts.