High-quality LiTaO3 thin films on silicon substrates are important for the application of silicon-based optoelectronic integration technology. In this article, single-crystalline LiTaO3 thin films were achieved by wafer-bonding and layer-transfer technology. Cross-sectional transmission electronic microscopy (TEM) and x-ray diffraction results indicate that the LiTaO3 thin films are single crystalline and have good structural quality. After hydrogen implantation and annealing, the surfaces of LiTaO3 samples were investigated in detail using optical microscopy and TEM. Results show that dose and implantation energy of hydrogen can both have effect on the cleavage of a thin surface section from a LiTaO3 wafer. (c) 2008 American Vacuum Society.