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The single-phase oxide PrBaCo2O6−δ and composites (100 − y)PrBaCo2O6−δ-yCe0.8Sm0.2O1.9 (y = 10–30 wt.%) were investigated as cathode materials for intermediate-temperature solid oxide fuel cells. The chemical compatibility, cation interdiffusion, thermal expansion and dc conductivity were studied. As a result, strong interdiffusion of Pr and Sm was found between PrBaCo2O6−δ and Ce0.8Sm0.2O1.9. This leads to only insignificantly decreasing thermal expansion coefficient of composite with increasing fraction of Ce0.8Sm0.2O1.9 and, thus, mixing PrBaCo2O6−δ with Ce0.8Sm0.2O1.9 does not improve thermal expansion behavior of the cathode material. Moreover, formation of poorly-conducting BaCeO3, caused by chemical interaction between the double perovskite and doped ceria, was shown to lead to pronounced drop in the electrical conductivity of the composite cathode material with increasing Ce0.8Sm0.2O1.9 content.