Epitaxial films of the perovskite, La0.8Sr0.2CoO3 (LSC), for SOFCs cathode were deposited on yttria-stabilized zirconia (YSZ) single crystals by pulsed laser deposition method. The films were characterized by thin-film X-ray diffraction measurement, atomic force microscopy (AFM), transmission electron microscope (TEM), and ac impedance spectroscopy. The film orientations depend on the substrate planes. The LSC films on the YSZ (100) and (111) substrates showed the (110) orientation with different twin structures, while those on the YSZ (110) had (100) and (112) orientations. Surface morphology of the films also depends on the substrate orientations. These films showed different electrode properties depending on the orientations. The relationships between the properties, the film orientations, surface morphology, and lattice misfit are discussed. (c) 2006 Elsevier B.V. All rights reserved.