precious metal-based electrocatalysts, such as platinum, iridium, or ruthenium, exhibit the outstanding catalytic performance, the costly price and scarcity confine their wide application. [6,7] Hence, it is compulsory to explore cost-effective, highly efficient, and long-life catalysts based on nonprecious metals. [8] Recently, transition metal-based electrocatalysts including transition-metal nitride, [9] phosphides, [10,11] and oxides [12] have been widely used for water splitting. Among them, transition metal sulfides included both layered MS 2 (such as MoS 2 , WS 2 ) and nonlayered M x S y (such as Co 9 S 8 , ZnS) are at the cutting edge owing to their structural diversity, electrical activity, and superior electrocatalytic performance. [13,14] Especially, molybdenum sulfide (MoS 2 ), which possesses 2D structure, stable physical, and chemical properties, has showed the superior HER activity in acidic and base media. [15] However, the HER performances of layered MoS 2 materials are still unable to overshine the Pt-based electrocatalysts because of poor conductivity and unexposed active sites. [1,16] To overcome these shortcomings, hybridizing MoS 2 with other active composites with high electrical conductivity to build heterostructure is a promising strategy, which exhibits synergistically promoted kinetics and tunes the electron configuration and possesses diverse active sites. [17] For instance, nickel sulfides (Ni x S y ) not only display good conductivity, but also are active for OER. [16,18] Many reports have illustrated that hybridizing two or more metal sulfides into a composite can significantly prompt the HER performance, even it provides a considerable solution to construct electrocatalysts for water splitting. [19,20] The promoted performance for such binary nanostructures could be primarily ascribed from modulated the electronic structure, their abundant reactive redox sites, synergistic interfaces, and customized conductivity. [21] For instance, Liu's group reported the yolk-shell MoS 2 /NiS-based materials for electrochemical water splitting only requiring a potential of 1.64 V in the base solution at 10 mA cm −2 . [22] Feng et al. constructed MoS 2 / Ni 3 S 2 nanocomposites on nickel foam generating ample interfaces. [23] Zhai et al. reported NiS 2 /CoS 2 /MoS 2 nanosheet arrays vertically grown on Ni foam by two facile procedures. [24] Nonetheless, the scarcity of inherent conductivity hinders these bifunctional nanohybrids to be the best replacement for precious-metal based electrocatalysts. [25] Consequently, structural construction and optimization linked to conductivity and performance are significant to attain advanced binary hybrids.