Designing an excellent acidic and alkaline general-purpose hydrogen evolution electrocatalyst plays an important role in promoting the development of the energy field. Here, a feasible strategy is reported to use the strongly coupled MoS2@sulfur and molybdenum co-doped g-C3N4 (MoS2@Mo-S-C3N4) heterostructure with transferable active centers for catalytic reactions in acidic and alkaline media. Research studies have shown that the unsaturated S site at the edge of MoS2 and the active N atom on the Mo-S-C3N4 substrate are, respectively, the active centers of acidic and alkaline hydrogen evolution reaction. Specifically, Mo-S-C3N4 is regarded as a synergistic catalyst for the active species MoS2 in acidic hydrogen evolution, while MoS2 acts as a co-catalyst when the alkaline active species are transferred to Mo-S-C3N4. The coordination of the electrons between the interfaces achieves a synergistic balance, which provides the optimal sites for the adsorption of the reactants. Such an electrocatalyst exhibits overpotentials of 193 and 290 mV at 10 mA cm-2 in 0.5 M H2SO4 and 1 M KOH, respectively, which was better than numerous previous reports. This research provides an outstanding avenue to realize multifunctional electrocatalysts.