Developing facile approaches for preparing efficient electrocatalysts is of significance to promote sustainable energy technologies. Here, we report a facile iron-oxidizing bacteria corrosion approach to construct a composite electrocatalyst of nickel–iron oxyhydroxides combined with iron oxides. The obtained electrocatalyst shows improved electrocatalytic activity and stability for oxygen evolution, with an overpotential of ∼230 mV to afford the current density of 10 mA cm−2. The incorporation of iron oxides produced by iron-oxidizing bacteria corrosion optimizes the electronic structure of nickel–iron oxyhydroxide electrodes, which accounts for the decreased free energy of oxygenate generation and the improvement of OER activity. This work demonstrates a natural bacterial corrosion approach for the facile preparation of efficient electrodes for water oxidation, which may provide interesting insights in the multidisciplinary integration of innovative nanomaterials and emerging energy technologies.