Layered double hydroxides (LDHs) are promising electrocatalysts for the oxygen evolution reaction (OER), but their stability and kinetics are limited by metal dissolution and lamellar structure ablation. This study introduces a bioinspired strategy using trimesic acid anchors to create sub-size NiFe-LDH nanosheets with enhanced OER performance. Operando spectroscopy and DFT calculations reveal that the superaerophobic surface facilitates O2 bubble release, while C-O-Fe bonding prevents metal dissolution. Uncoordinated carboxylates act as proton ferries, accelerating OER kinetics. This approach offers a pathway to improve OER stability and dynamic performance.