requires 58, 70, and 129 mV in alkaline, acid, and neutral media, respectively, to reach 10 mA cm -2 , which also presents fast reaction kinetics and high long-term stability. The experimental and density functional theory (DFT) results verify that the abundant active heterostructure in Super-Co 3 S 4 /P-WS 2 /Co 9 S 8 can not only provide Pt-like H*-adsorption Gibbs free energy (ΔG H* ) but also promote the H 2 O adsorption and dissociation kinetics for all-pH HER. Moreover, the collaboration of favorable metallic components and special nanoarray morphology can also strengthen the electric conductivity for electron transfer and promote the maximum exposure of active heterointerfaces for mass transport in electrocatalysis. The interesting strategy herein is expected to inspire the future design of advanced metal sulfide-based heterostructures for energy storage and conversion.