NiFe‐based hydroxides are well‐established as efficient electrocatalysts for the oxygen evolution reaction (OER) in alkaline purified water. However, they usually degrade rapidly in seawater electrolysis because of concentrated Cl− anions in seawater. In this work, a facile approach utilizing an ultrafast dipping method is presented to fabricate durable and scalable NiFe hydroxides, enhanced by interfacial akaganéite FeOOH for seawater splitting. This study reveals significantly improved electrocatalytic stability of NiFe hydroxides at an ampere‐level current density of 1000 mA cm−2 for 100 h in alkaline seawater. It is realized by the formed FeOOH in a specific akaganéite phase whose lattice tunnels are well filled by intrinsic Cl− anions, that serve to electrostatically repel corrosive chlorides in electrolyte. This anionic design also provides superior corrosion protection for other active metal‐based OER electrocatalysts when deployed in alkaline purified water and allows for facile scaling up of the anode, facilitating the practical utilization for seawater electrolysis.