Thin films of carbon nitride were deposited using pulsed laser deposition techniques both with and without an atomic nitrogen source. In situ characterization of chemical composition and atomic bending were studied using scanning Auger, x-ray photoelectron spectroscopy, and electron energy-loss spectroscopy. The influence of growth parameters including substrate temperature, substrate bias, nitrogen partial pressure, and atomic nitrogen on the film composition were studied. Nitrogen content x for CNx films ranged from 0.3 to 0.6 (25-40 at. % nitrogen). Time-of-flight mass spectrometry of the species ejecting from a nitrided carbon target was performed. Neutrals of CN4 and C3N4 clusters and positive ions of CxNy clusters were observed in addition to carbon neutral and positive ion clusters.