alkaline electrolyzers are still inefficient due to the existence of large overpotentials induced from the sluggish kinetics of hydrogen and oxygen evolution reactions (HER and OER), thus leading to high electric power consumption and high costs for hydrogen production. [1][2][3] Therefore, it is of great importance to develop advanced HER and OER electrocatalysts to accelerate the kinetics and greatly reduce the overpotentials for water splitting. However, the current state-of-the-art electrocatalysts for water splitting are mainly based on noble metals or noble metal-related materials (e.g., Pt, Pd, IrO 2 , and RuO 2 ), which greatly restrict the large-scale application of industrial water electrolysis due to the high price and low reserves of these materials. In this regard, developing low-cost and earthabundant electrocatalysts with high activity and good stability is crucial for increasing the energy conversion efficiency of water splitting. [4][5][6] In addition, considering the system simplification and cost-cutting in practical commercialization, constructing an advanced bifunctional electrocatalyst with outstanding OER and HER activities in the same media is technologically imperative. [7][8][9] Although some progress has been made during the past few years, it still remains challenging to develop bifunctional non-noble metal-based catalysts with exceptional performance for overall water splitting.To date, a variety of non-noble and earth-abundant materials have been reported as potential catalysts for HER or OER Alkaline water electrolysis is an advanced technology for scalable H 2 production using surplus electricity from intermittent energy sources, but it remains challenging for non-noble electrocatalysts to split water into hydrogen and oxygen efficiently, especially for tungsten disulfide (WS 2 )-based catalysts. Density functional theory calculations in combination with experimental study are used to establish a multi-site engineering strategy for developing robust WS 2 -based hybrid electrocatalyst on mesoporous bimetallic nitride (Ni 3 FeN) nanoarrays for bifunctional water splitting. This ingenious design endows the catalyst with numerous edge sites chemically bonded with the conductive scaffold, which are favorable for water dissociation and hydrogen adsorption. Benefiting from the synergistic advantages, the N-WS 2 /Ni 3 FeN hybrid exhibits exceptional bifunctional properties for hydrogen and oxygen evolution reactions (HER and OER) in base with excellent large-current durability, requiring 84 mV to afford 10 mA cm −2 for HER, and 240 mV at 100 mA cm −2 for OER, respectively. Assembling the catalytic materials as both the anode and cathode to construct an electrolyzer, it is actualized very good activities for overall water splitting with only 1.5 V to deliver 10 mA cm −2 , outperforming the IrO 2 (+) //Pt (−) coupled electrodes and many non-noble bifunctional electrocatalysts thus far. This work provides a promising avenue for designing WS 2 -based heterogeneous electrocatalysts for water el...