Amorphous carbon nitride films (a-CN.) were synthesized by using single ion beam sputtering of a graphite target in argon and nitrogen sputtering gases. This thin film could be used as a novel photovoltaic material. The films were characterized with the technique of laser Raman, spectroscopic ellipsometry and electron spin resonance spectrometer (ESR). In this paper we report the effects of ion impacting and nitrogenation on the microstructure, density of defect states, bonding character, optical and photovoltaic properties. Effective decreasing of intensity of the ESR signal and formation of C-N bonding were observed, which could be attributed to the increment of the impinging ions on the growing films. The nitrogenation of a-CNx films could decrease the Tauc optical gap (0.62-0.86eV) and the intensity of ESR signal, increase photon absorption coefficient of the films (106-10 4 cm').The primary photovoltaic values of the devices having Schottky structure of ITO/CN./Al are I, 1.56 il A/cm 2 and Vo. 250 mV, respectively, when exposed to AM1.5 illumination ( 100oW/cm 2