In the present study, amorphous hydrogenated carbon (a-C:H) thin films were successfully prepared on Corning glass and stainless steel (SS) substrates via spin coating technique from a polymeric solution through thermal decomposition. For the first time, the effects of annealing atmospheres consisting of argon, nitrogen, and air on the structural, vibrational, and morphological properties of the films deposited on Corning glass substrates were investigated by Raman spectroscopy, FTIR spectroscopy, AFM, and FE-SEM. The surface corrosion tests of uncoated and a-C:H coated stainless steel (SS) substrates were evaluated by potentiodynamic polarization analysis. The results indicated that diamond like carbon (DLC) character, surface roughness as well as surface corrosion resistance behavior of the specimens depend on the type of annealing atmosphere. The films annealed under N2 exhibited smoother surface with lower sp3 fraction, while annealing in Ar caused to increase roughness with the higher sp3 fraction. It was also found that in all the samples, a-C:H coating acted as a proper barrier between the substrate and the corrosive medium. Especially, Ar-annealed a-C:H coating could be a candidate as a surface corrosion-resistance coating due to low surface corrosion current density and broad passivity region of anodic polarization branch. Furthermore, the fabricated a-C:H thin films involved with high film thickness controllability and good adhesion without needing the interlayer materials.