Carbonitride thin films have been deposited on silicon substrate by the irradiation of energetic nitrogen ions emanated from dense plasma focus device. The carbon ions are ablated by the irradiation of relativistic electrons from the insert material (graphite) placed at the anode tip. The x-ray diffraction analysis demonstrates that a polycrystalline thin film consisting of various compounds such as Si3N4, SiC, and C3N4 is formed on the silicon (100) substrate. Crystallinity of different compounds decreases with the increase in angular positions (0 degrees, 10 degrees, and 20 degrees). Raman spectroscopy shows the appearance of graphitic and disordered bands with silicon nitride and silicon carbide indicating the formation of carbonitride. Raman spectra also indicate that broadening of bands increases with the increase in focus deposition shots, leading to the amorphization of the thin film. The amorphization of the thin films depends on the ion energy flux as well as on the sample angular position. The scanning electron microscopy exhibits the damaging of the substrate surface at 0 degrees angular position. The microstructure shows the tubular shape for higher ion dose (40 focus shots). At 10 degrees angular position, a two phase phenomenon is observed with the ordered phase in the solid solution. A smooth and uniform surface morphology showing a small cluster is observed for the 20 degrees angular position.