The study presents a novel strategy for highly stable and efficient brine oxidation at high current densities using CoFeAl-layered double hydroxide (CoFeALDH) anodes. The anodes are synthesized through a one-step hydrothermal method and exhibit excellent oxygen evolution reaction (OER) activity, maintaining stable catalytic performance for 350 hours at 2 A cm⁻² in 6-fold concentrated seawater. The Al³⁺ ions in the electrode are etched off by OH⁻ during the OER process, forming M³⁺ vacancies that enhance OER activity. Additionally, self-generated Al(OH)₃⁻ adsorbs on the anode surface, improving stability by enriching OH⁻ and repelling Cl⁻ through Coulombic forces. This mechanism ensures efficient and stable oxidation in concentrated brine at 1.0–2.0 A cm⁻² current densities for more than 350 hours. The feasibility of the CoFeALDH anodes is demonstrated through the operation of a membrane electrode assembly (MEA) at 1 A cm⁻² for 500 hours, highlighting their potential for practical applications in continuous seawater electrolysis.The study presents a novel strategy for highly stable and efficient brine oxidation at high current densities using CoFeAl-layered double hydroxide (CoFeALDH) anodes. The anodes are synthesized through a one-step hydrothermal method and exhibit excellent oxygen evolution reaction (OER) activity, maintaining stable catalytic performance for 350 hours at 2 A cm⁻² in 6-fold concentrated seawater. The Al³⁺ ions in the electrode are etched off by OH⁻ during the OER process, forming M³⁺ vacancies that enhance OER activity. Additionally, self-generated Al(OH)₃⁻ adsorbs on the anode surface, improving stability by enriching OH⁻ and repelling Cl⁻ through Coulombic forces. This mechanism ensures efficient and stable oxidation in concentrated brine at 1.0–2.0 A cm⁻² current densities for more than 350 hours. The feasibility of the CoFeALDH anodes is demonstrated through the operation of a membrane electrode assembly (MEA) at 1 A cm⁻² for 500 hours, highlighting their potential for practical applications in continuous seawater electrolysis.