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A new heterostructured (La,Sr)₂FeO_4−δ (LSF₂₁₄)-La_0.8Sr_0.2FeO_3−δ (LSF₁₁₃) electrode has been synthesized to improve the oxygen reduction reaction (ORR). This new materials system was fabricated by the deposition of Sr(NO₃)₂ into the LSF₁₁₃ framework followed by subsequent heat treatment, resulting in a new three-dimensional (3D) LSF₂₁₄-LSF₁₁₃ heterostructured electrode. This material system consists of a with Ruddlesden–Popper (R–P) LSF₂₁₄ phase formed on the surface of the LSF₁₁₃ framework. The ORR activity has been enhanced by 1 order of magnitude using the LSF₂₁₄-LSF₁₁₃ heterostructured electrode. The ORR enhancement was the result of higher catalytic activity of the LSF₂₁₄ phase and a mismatch in the lattice parameter between LSF₂₁₄ and LSF₁₁₃ regions which results in oxygen molecule adsorption and oxygen vacancy formation become more favered. Impedance …