Electrode/electrolyte composite materials for all-solid-state lithium secondary batteries were prepared by coating the 80Li(2)S center dot 20P(2)S(5) (mol%) solid electrolyte onto LiCoO2 electrode particles using the pulsed laser deposition method. Cross-sectional transmission electron microscopy images showed that the solid electrolyte layer was formed on the LiCoO2 particles. The all-solid-state cell using the LiCoO2 particles coated with the solid electrolyte was charged and discharged, and exhibited good cycle performance. This suggests that the electrolyte coatings provide a lithium-ion conduction path to LiCoO2, and the technique is effective in the development of all-solid-state cells. (C) 2010 The Electrochemical Society. [DOI: 10.1149/1.3376620] All rights reserved.