Self‐supported Fe2P/Co2N porous heterostructure arrays are in situ constructed with abundant iron sites exposing at the surface, which presents superb bifunctional catalytic activity for hydrogen and oxygen evolution reactions in base, substantially expediting the overall water splitting at 500 mA cm−2 with only 1.663 V, prominently superior to IrO2(+)//Pt(−) coupled electrodes and most of non‐noble bifunctional electrocatalysts. Abstract Alkaline water electrolysis is a commercially viable technology for green H2 production using renewable...