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[Display omitted] • Compositional regulation by introducing MoS 2 provides rich H adsorption sites. • Internal electronic regulation in heterostructure accelerates the RDS in OER process. • MnCo 2 S 4 @MoS 2 employed as a bifunctional catalyst for efficient hydrogen production. • Operating stably in industrial condition with structural reconstruction at the anode. • The electron redistribution and reaction pathways are explained by DFT calculations. It remains to be challenging to develop bifunctional catalysts for overall water splitting (OWS) with high activity and durability at large current density. In an attempt to overcome this bottleneck, unique MnCo 2 S 4 hexagonal stars covered with MoS 2 nanosheets were in-situ grown on nickel foam (NF) to obtain MnCo 2 S 4 @MoS 2 /NF heterostructure with optimized composition and local electronic structure in this work. When employed as a bifunctional catalyst, it only needs low overpotentials of 208 and 332 mV in 6.0 M KOH to drive 1000 mA cm−2 with small Tafel slopes of 56.8 and 75.6 mV dec-1 for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. In addition, MnCo 2 S 4 @MoS 2 /NF showed remarkable stability in simulated industrial conditions, operating stably for 50 h at 1000 mA cm−2 without any attenuation for HER/OER. Thus, the MnCo 2 S 4 @MoS 2 /NF can function as a bifunctional electrocatalyst for OWS, only requiring 1.795 V to afford 1000 mA cm−2 with splendid stability. The improved performance is ascribed to dual electric and compositional regulation, which endow MnCo 2 S 4 @MoS 2 /NF with rich active sites and heterointerfaces, thereby promoting electron transfer and boosting the reaction kinetic. Furthermore, density functional theory (DFT) calculations reveal that the construction of heterostructure can help regulate intrinsic electronic structure, resulting in accelerated reaction kinetics. This work provides a reasonable and meaningful method for boosting industrial green hydrogen production. [ABSTRACT FROM AUTHOR]