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Boron carbonitride and boron nitride films were grown by plasma-enhanced chemical vapor deposition using trimethylamineborane and its mixtures with ammonia, hydrogen, or helium. The effects of the starting-mixture composition and substrate temperature on the chemical composition of the deposits was studied by ellipsometry, scanning microscopy, IR spectroscopy, Raman scattering, and x-ray photoelectron spectroscopy. The results indicate that the initial composition of the gas mixture, the nature of the activation gas, and substrate temperature play a key role in determining the deposition kinetics and the physicochemical properties of the deposits. Depending on these process parameters, one can obtain h-BN, h-BN + B4C, or BCxNy films.