The development of efficient and stable bifunctional non-noble metal catalysts for overall water splitting remains an important challenge. In this study, graphene-like carbon encapsulated Ni/Mo2C catalysts were prepared by hydrothermal and high temperature pyrolysis method. Due to the synergistic effect of Ni and Mo2C, the HER and OER performance of the catalysts was improved. The catalyst achieved an overpotential of 131 mV and a Tafel slope of 50.44 mV·dec-1 for the hydrogen evolution reaction (HER) in 0.5 M H2SO4, and an overpotential of 330 mV and a Tafel slope of 59.64 mV·dec-1 for the oxygen evolution reaction (OER) in 1.0 M KOH. The low overpotential and fast reaction kinetics make the water decomposition process more direct and efficient. This study provides a new approach for designing bifunctional catalysts for efficient water electrolysis applications.