MOF ‐Derived Superaerophobic Ni‐ CoOOH Nanosheet Anchored on Stretched Carbon via In Situ Morphology Reconstruction for Durable Oxygen Evolution

The efficiency of water electrolysis is heavily affected by bubble adhesion on electrodes, which blocks active sites and increases resistance. Surface structural engineering facilitates bubble detachment and improves gas release, yet challenges remain in achieving scalable fabrication while maintaining both high conductivity and superaerophobicity. Herein, we propose a metal‐organic framework (MOF)‐derived electrocatalyst that undergoes in situ electrochemical reconstruction, in which Ni‐doped Co nanoparticles embedded in a carbon framework expand and transform into vertically aligned nanosheets. This reconstruction process not only produces a superaerophobic/superhydrophilic interface that enables bubble‐free oxygen release and continuous active‐site exposure, but also induces tensile strain in the carbon skeleton, disrupting N‐C bonds to enhance the electrical conductivity of CoOOH. Meanwhile, Ni doping optimizes the *OOH adsorption free energy, thereby accelerating the rate‐determining step of the oxygen evolution reaction. Electrochemical studies confirm low overpotentials, efficient charge transfer, and long‐term durability, while density functional theory calculations elucidate the synergistic effects of strain engineering and electronic modulation. By exploiting the inherent structural tunability and porosity of MOF precursors, this design demonstrates the potential of MOF‐derived catalysts as a versatile and scalable platform for integrating surface morphology control with bubble dynamics regulation, offering valuable guidance for high‐performance water splitting systems.