High activity trifunctional non-noble electrocatalysts, targeting oxygen reduction reaction (ORR), hydrogen evolution reaction (HER), and oxygen evolution reaction (OER), are rationally designed by integrating the merits of both Co9S8 nanoparticles and carbons nanosheets. Herein, Co9S8 loaded with S, N co-doped carbon core–shell catalyst (Co9S8@SNC) was reasonably designed and synthesized by using the strong coordination effect between Co2+ and CS at the molecular level. The significant synergistic effect between the S, N co-doped carbon shell and Co9S8 core endows the catalyst with excellent catalytic performance for ORR, HER, and OER reactions. The carbon shell enhances the conductivity of the hybrid material, while the Co9S8 core provides the main catalytic active sites. More specifically, the half-wave potential for ORR is 0.846 mV, and the overpotential at 10 mA cm−2 for OER and HER are 320 mV and 170 mV, respectively. To test its practical application, zinc-air battery assembled by Co9S8@SNC shows a high power density of 239 mW cm−2, excellent rechargeability, and long cyclic stability. This work provides a promising and extensible method to in-situ synthesize core–shell metal sulfides loaded S, N co-doped carbon composites, which can be a promising candidate for electrocatalytic material in energy storage and conversion devices.