On the basis of the rich reserves of elements on the earth, the development of highly efficient and durable hydroelectric catalysts is of great significance for solving environmental pollution and energy crises. Herein, moss-like iron phosphide particles on a nickel foam substrate were fabricated through a combined electrodeposition and solvothermal method and exhibited excellent electrocatalytic performance for overwater electrolysis in alkaline media. The obtained FeP-350/NF showed excellent oxygen evolution reaction and hydrogen evolution reaction performance with low overpotentials of 388 and 413 mV at 100 mA cm −2 , respectively. Assembling FeP-350/NF into a two-electrode water electrolysis device only needs 1.54 V to achieve a current density of 10 mA cm −2 , and there is no sign of decay in the electrolysis of water for 24 h, implying that the material has potential practical application value. Further, MIL-88A has shown good application prospects in many environmental protection fields. MIL-88A is a metal−organic framework (MOF) that is particularly easy to synthesize, and the cost of raw materials is particularly low. Most importantly, MIL-88A is nontoxic to organisms. This method with MIL-88A offers a facile and green strategy for designing not only phosphide based material but also metal oxide-based highly active bifunctional electrocatalysts system and paves the way for the future development of energy conversion systems.