LiNb1-xTaxO3 films with x = 0.3-0.7, epitaxial orientation and good crystallinity were prepared by using thermal plasma spray CVD. Mixtures of metalorganic solutions containing lithium-niobium and lithium-tantalum alkoxides were used as liquid source materials. Preferentially (001)-oriented LiNb1-xTaxO3 films were fabricated on sapphire (001) substrates with deposition rates up to approximately 6 nm/s, which was approximately 100 times as fast as those of most conventional vapor phase deposition methods. LiNb1-xTaxO3 films with x = 0.5 achieved a (006) rocking curve full-width at half-maximum value of 0.15-0.20 degrees, which is comparable with those of LiNbO3 and LiTaO3 films grown by other conventional deposition techniques. This is the first success in preparing LiNb1-xTaxO3 films with x > 0.33, good crystallinity and high (001) orientation.