Abstract Bifunctional transition metal electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are key to sustainable water splitting and are widely studied. In line with this, the present study designs and tests an electrocatalyst consisting of an amorphous iron vanadium layer on anti‐perovskite nickel zinc nitride (FeV_NiZnN). Because of the synergistic association between the amorphous FeV layer and anti‐perovskite NiZnN, the formation of a hydroxide/metal nitride interface during the course of electrochemical experiments, and exposure of a higher number of active sites, the proposed FeV_NiZnN catalyst demonstrates an effective and durable bifunctional water‐splitting performance. In particular, the as‐prepared FeV_NiZnN catalyst achieves 201 mV@10 mA cm −2 for the OER and 115 mV@50 mA cm −2 for the HER in an alkaline solution, representing excellent water‐splitting activity. The water‐splitting performance of FeV_NiZnN is also tested in a two‐electrode system, recording a current density of 50 mA cm −2 at 1.63 V without iR compensation and exhibiting highly durable long‐term operation. The proposed catalyst also demonstrates a low operating voltage and high stability in anion exchange membrane‐based water electrolysis. The FeV amorphous layer on anti‐perovskite NiZnN promotes both HER and OER, offering insights into the design of efficient bifunctional electrocatalysts for water splitting.