Fe‐Mediated Electron Transfer in an Amorphous/Crystalline Heterostructure Boosts Oxygen Evolution Reaction

While in‐situ growth strategies can overcome the mechanical instability of power catalysts, composite construction via composition control limits atomic orbital and intermediate modulation, restricting catalytic enhancement. Controllable tuning of the interfacial environment and electronic structure to boost intrinsic activity remains a critical challenge. In this study, a hierarchical Ni 3 S 2 –Fe/NF catalyst was constructed through interfacial engineering. Spectroscopic characterization reveals that the amorphous Fe interlayer facilitates efficient intercomponent charge transfer via interfacial polarization‐induced electron redistribution, functioning as an electron‐conducting bridge. Furthermore, the optimized catalyst exhibits an order‐of‐magnitude of longer stability than most recently reported Ni 3 S 2 ‐based catalysts, meeting rigorous durability requirements for practical applications. This study highlights the crucial role of interfacial electronic modulation between Fe and Ni 3 S 2 , where the amorphous Fe interlayer acts as an electron‐conducting bridge to enhance oxygen evolution reaction (OER) performance, offering valuable insights into heterostructure design for efficient electrocatalysis.