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A series of single-phase double perovskite Pr1-xGdxBaCo2-yFeyO5+δ (x = 0, 0.5 and 1, 0 ≤ y ≤ 1) materials were engineered through A/B site co-doping strategy to improve the mechanical, electrical and electrochemical properties as potential cathode materials for the application of intermediate solid oxide fuel cells (IT-SOFCs). The corresponding thermochemical stability, thermal expansion behavior, electrical conductivity and cathodic polarization resistance of the materials were systematically investigated. It was found that the A-site dual lanthanide doped Pr0.5Gd0.5BaCo2O5+δ (PGBCO) exhibits improved electrical conductivity, reduced thermal expansion, and comparatively low electrochemical polarization resistance versus single lanthanide double perovskite, PrBaCo2O5+δ (PBCO) and GdBaCo2O5+δ (GBCO) materials. Further investigation on the effect of B-site Fe-doping on Pr0.5Gd0.5BaCo2-yFeyO5+δ (PGBCF-y, 0 ≤ y ≤ 1) reveals that all the PGBCF-y compositions exhibit excellent chemical stability with Gd-doped ceria (GDC) at operating temperatures not higher than 1 100 °C. Besides, doping of Fe in B-site can effectively reduce the thermal expansion coefficients (TECs) of the Pr0.5Gd0.5BaCo2O5+δ ceramics at 30–1 000 °C. And the electrochemical impedance spectra (EIS) results show that the PGBCF-y|GDC| PGBCF-y symmetric cells have acceptable low area specific polarization resistances. Further examination of the cathodic polarization and characteristic capacitance from the AC impedance spectra by employing the relaxation time distribution (DRT) method demonstrated that charge transfer is the dominating sub-process for the oxygen transport through the materials.