Hydrogenated amorphous carbon films were prepared from CH4, H2, and Ar mixtures by plasma enhanced chemical vapor deposition. Films with various physical properties resulting from various deposition conditions were utilized for this study. The varying deposition parameters included H2flow rates, Ar flow rates, total pressures, substrate temperatures, and power densities. A systematic study regarding the relationship between deposition conditions and the microstructures, optical, and thermal properties was conducted. Furthermore, how the optical and thermal properties related to the microstructures was analyzed. Fourier transform infrared spectroscopy was employed in this paper for determining the hydrogen concentration and the amounts of tetrahedral and trigonal bondings associated with C—H bond and their relative ratio while the optical properties were measured by optical spectrophotometer. Additionally, photothermal deflection spectroscopy was applied for the measurements of thermal diffusion length.