Framework materials, particularly metal-organic frameworks (MOFs), have emerged as versatile platforms for multifunctional applications due to their tunable structures and properties. In this study, a series of bimetallic ZnRuMOFs with dual-crystalline phase structure was designed and synthesized. This unique dual-crystalline bimetallic MOF configuration enables intramolecular autocatalysis and selective oxygen reduction reaction (ORR). By utilizing endogenous dissolved O