sulfide (TMS) catalysts in alkaline environments, as attested with a lower overpotential of 337 mV at 10 mA cm −2 and a smaller Tafel slope of 77 mV dec −1 . Meanwhile, a Zn−air battery based on Ni 3 S 2 −Co 9 S 8 /NCA + Pt/C achieves a large power density of up to 256 mW cm −2 (and 193 mW cm −2 ), small charge/discharge voltage gap, and good cycling stability, notably better than the conventional RuO 2 + Pt/C-based Zn−air batteries. These excellent electrocatalytic properties are mainly attributed to the distinct hierarchical porous structure and interfacial synergy between the Ni 3 S 2 and Co 9 S 8 nanoparticle structure with rich defects, facilitating the mass transport and high graphitization degree beneficial for electron mobility. It is envisioned that the research provides a novel approach for the exploration of marine biomass as an electrocatalyst.