Tracking <i>in situ</i> transformation of metal–organic frameworks into layered double hydroxides during synthesis and alkaline water oxidation through <i>operando</i> mechanistic studies

, are integrated with DFT insights to construct a unified picture of intermediate species, structural dynamics, and thermodynamic stability. We further discuss how defect chemistry, metal-oxygen flexibility, and dissolution-reprecipitation behaviour shape durability under harsh OER conditions. The perspective concludes with key challenges and future opportunities for mechanistically guided design of next-generation MOF-derived LDH electrocatalysts.