Raman spectra of a-C:H thin films deposited with an unbalanced magnetron sputtering system showed that the G peak shifted to a higher wavenumber as the target power density increased and ID/IG ratio increased from 0.902 to 1.012. Moreover, the transmittance of a-C:H films fabricated at 60 nm tended to decrease with increasing target power density; at 550 nm in the visible light region, the transmittance decreased from 69% to 58%. The rms surface roughness values of the a-C:H thin films decreased with increasing target power density, and varied from 1.11 nm to 0.71 nm. In order to achieve efficient light trapping, the light scattering at the rough interface must be enhanced. Consequently, the surface roughness of the thin film will decrease with the target power density. Further, the refractive index and reflectivity of the a-C:H thin films increased with increasing target power density; however, the Brewster angle decreased with the target power density. Hence, dye-sensitized solar cells using an a-C:H antireflective coating increased the CE, VOC, and JSC by approximately 8.6%, 5.5%, and 4.5%, respectively.