ABSTRACT Constructing stable, molecularly defined active interfaces on cost‐effective oxide supports is a pivotal yet unmet challenge in oxygen evolution reaction (OER) electrocatalysis, as conventional sacrificial or indirect strategies preclude direct control over the functional interface where catalysis unfolds. Herein, we demonstrate this concept on spinel iron oxide, achieving a robust Fe‐(O,N)‐C coordination shell on Fe 3 O 4 via dual‐ligand capture‐reorganization. Density functional theor