High quality lithium niobate (LiNbO 3 ) epitaxial thin films have been grown on c-plane sapphire and LiTaO3 substrates by solid-source MOCVD using the tetramethyl-heptanedionate sources, Li(thd) and Nb(thd) 4 . Phase content was controllable, and stoichiometric films were reproducibly deposited over a broad temperature range from a Li(thd)-rich source. Using sapphire substrates, with which the occurrence of multiple in-plane orientations is typically a problem, LiNbO 3 films with only one in-plane orientation could be prepared within a narrow range of growth conditions. XRD rocking curve FWHM values as low as 0.04', and optical waveguiding losses near 2dB/cm (1200A thick film, TM 0 mode, 632.8nm) were obtained. However, film thicknesses on sapphire were limited to 2000A because of cracking caused by the large thermal expansion mismatch, and in such thin films, optical confinement is poor.In contrast, LiTaO 3 has almost same lattice constants and thermal expansion coefficients as LiNbO 3 , making it a potentially superior substrate material. Lithium niobate films up to 6000A were successfully deposited on LiTaO 3 substrates without cracking. Film quality was greatly improved, with FWHM values as low as 0.01', and rms surface roughness less than 10 A. Preliminary optical waveguiding losses less than 6 dB/cm for the TEO mode have been achieved.