ZnO1-xSx thin film has been successfully fabricated by pulsed laser deposition. The electrochemical properties are investigated by charge/discharge measurement and cyclic voltammograms. X-ray diffraction, x-ray photoelectron spectroscopy, high-resolution transmission electron microscopy, and selected area electron diffraction measurements are employed to explore their electrochemical reaction mechanism with lithium. Among all the ZnO1-xSx compounds, ZnO0.28S0.72 shows the best electrochemical performance with a large reversible specific capacity around 650 mAh/g and an excellent capacity retention. The electrochemical reaction mechanisms of the film in the charging and discharging processes involve the reversible decomposition/formation of ZnO1-xSx and alloying/dealloying of ZnLi. (C) 2011 The Electrochemical Society. [DOI:10.1149/1.3532037] All rights reserved.