The present research addresses the synthesis of carbon materials thin films by RF-PECVD in N2/CH4 gas mixture. Carbon materials film was formed at 40/48 sccm of CH4/N2 of the total gas flow rate ratio CH4/CH4+N2 = 0.45 and 200/100 W HF/LF power at a deposition temperature of 350 oC and 1000 mTorr pressure. Then, post-annealing of carbon materials film took place at 400 oC by means of RTA under N2 flow. The formation of carbon nanostructures was investigated by scanning electron microscopy, energy dispersive X-ray, Raman spectroscopy, and atomic force microscopy, respectively. AFM shows that the films consisted of nanocrystalline grains. The surface morphology and structural characteristics of materials were studied as a gas flow function and substrate temperature. EDX results indicated the carbon presence, and Raman spectroscopy analysis revealed two broad bands: D-band 1381.64 cm−1 and G-band 1589.42 cm−1. The temperature-dependent post-annealing of carbon materials plays a key role in the graphite crystallites growth at high substrate temperatures. Our results indicate carbon materials incorporation for laser diode applications.