The efficient non-noble metal-based bifunctional electrocatalyst for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) has attracted great interest, which is highly significant to enhance the efficiency of hydrogen production from water electrolysis. Herein, inspired by the appropriate hydrogen adsorption free energy of transition metal alloy and the strong corrosion resistance of phosphide in alkaline electrolyte, carbon compound NiFeMo-P anchored on nickel foam (NiFeMo-P-C) is obtained by simple one-pot hydrothermal and subsequent hydrogen reduction treatment. Remarkably, the NiFeMo-P-C exhibits excellent bifunctional electrocatalytic performances toward HER and OER with low overpotentials of 87 and 196 mV at 10 mA·cm^–2, respectively. Moreover, the electrolyzer using NiFeMo-P-C as both cathode and anode only requires a cell voltage of 1.50 V to reach a current density of 10 mA·cm^–2, along with an outstanding long-term stability for 50 h. The synergistic effect among alloys and phosphide, partially broken hollow morphology and porous nickel foam substrate jointly impart NiFeMo-P-C high electrocatalytic activity and superior durability.