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Developing highly efficient, cost effective and durable bifunctional electrocatalyst remains a key challenge for overall water splitting. Herein, a bifunctional catalyst CoP₂-Mo₄P₃/NF with rich heterointerfaces was successfully prepared by a two-step hydrothermal-phosphorylation method. The synergistic interaction between CoP₂ and Mo₄P₃ heterogeneous interfaces can optimize the electronic structure of active sites, leading to the weak adsorption of H on the Mo sites and the increased redox activity of the Co site, resultantly improving the HER/OER bifunctional catalytic activity. The synthesized CoP₂-Mo₄P₃/NF catalyst exhibits excellent electrocatalytic activity in 1.0 M KOH with low overpotentials of 77.6 and 300.3 at 100 mA cm⁻² for HER and OER, respectively. Additionally, the assembled CoP₂-Mo₄P₃/NF||CoP₂-Mo₄P₃/NF electrolyzer delivers a current density of 100 mA cm⁻² at a cell voltage of 1.59 V and remains stable for at least 370 h at 110 mA cm⁻², indicating the potential application prospective in water splitting.