To push forward the hydrogen energy technology, it is crucial to develop a highly active catalyst for the application of water splitting. Nevertheless, many electrocatalysts suffer from functional limitations, making them unsuitable for both anode and cathode applications. Therefore, the utilization of bifunctional electrocatalysts is necessary to overcome this limitation. In this study, we have reported a bifunctional CoMoP-FexP/NF catalyst with favorable electrocatalytic performance toward hydrogen evolution reaction/oxygen evolution reaction (HER/OER). Balanced amorphous/crystalline heterophase endows CoMoP-FexP/NF with more exposed active sites. In addition, the superhydrophobic nature of CoMoP-FexP/NF helps to improve the contact with electrolyte. Following conditional optimization, CoMoP-FexP/NF requires only an overpotential of 85.6 mV to achieve a current density of 10 mA cm−2 for HER, and 249.6 mV for a current density of 20 mA cm−2 for OER. A water-splitting electrolyzer comprising CoMoP-FexP/NF requires a low cell voltage of 1.56 V to achieve a current density of 10 mA cm−2. This study provides valuable insights into designing bifunctional electrocatalysts and replacing noble metallic materials to enhance hydrogen production from water splitting.