The development of cost-effective and high-performance bifunctional catalysts for overall water splitting is crucial for achieving sustainable clean energy. In this study, a metal/carbide hybrid (NiFeMo/NiFeMoCx) was prepared through fast and facile cathodic plasma electrolytic deposition. Due to the synergistic effect between the metal and carbide, NiFeMo/NiFeMoCx exhibited high activity in both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER), with overpotentials of 230 mV and 60 mV at 10 mA cm−2, respectively. In addition, robust stability was demonstrated during the overall water splitting (1.52 V at 10 mA cm−2, with little degradation after 18 h of catalysis). This work provides a useful strategy for designing advanced water splitting catalysts for real application.