Single crystal thin films of LiNb0.5Ta0.5O3 were prepared on (001)LiTaO3 and (001) LiNbO3 substrates by a thermal plasma spray CVD process using metalorganic precursors. The composition and epitaxial quality of the films, deposited at the growth rate of 20-400 nm/min, were evaluated by transmission electron microscopy and X-ray diffractometry. The surface morphology of the films was characterized by atomic force microscopy in relation to the deposition temperature and the substrate surface conditions. (C) 2002 Elsevier Science B.V. All rights reserved.