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Lithium niobate thin films were deposited on (0001) sapphire using metalorganic chemical vapor deposition. An organometallic compound, formed by reaction of lithium dipivaloylmethanate and niobium(V) ethoxide, was used as a single‐source precursor. The epitaxial nature of the films was established by x‐ray diffraction and Rutherford backscattering analyses (RBS).