The properties of amorphous hydrogenated carbon nitride (a-C:N:H) materials create the potential for a variety of commercial applications. Plasma-enhanced chemical vapor deposition (PECVD) provides a convenient means of creating thin a-C:N:H films, but the chemistry that dominates the deposition remains unclear. The CN radical likely plays a role in the process; here, CH 3 CN was used as a single-source precursor for the generation of CN radicals and the PECVD of a-C:N:H films. Several plasma diagnostic techniques were used in an effort to clarify important deposition mechanisms, with special attention given to the role of CN radicals in the deposition process. Gas phase characterization methods, including laser-induced fluorescence (LIF) and optical emission spectroscopy (OES), provide insight into the formation and gas phase properties of CN(g). In addition, the behavior of CN at the plasma-surface interface was probed using the imaging of radicals interacting with surfaces (IRIS) technique. Results suggest that CN reacts at surfaces with high probability and little regard to changes in important deposition parameters. Finally, the growth rate and morphology of these films were characterized to investigate the role of substrate temperature in the deposition process.