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The addition of Si to amorphous hydrogenated C (Si-AHC) films improves their durability while maintaining their desirable high-hardness, low-friction, and low-wear characteristics. The effects of added Si on the microstructure of Si-AHC films grown by a plasma-enhanced CVD process were studied using Raman scattering and spectroscopic ellipsometry. The relative intensity of D-band to G-band observed in Raman spectra of aC reflects the average size of sp^ 2 clusters as well as the sp^ 2/sp^ 3 carbon bonding ratio. Using this metric for the Si-AHC films we find that both the sp^ 2 cluster size and the sp^ 2/sp^ 3 C-bonding ratio decrease with added Si. Lorentz parameters derived from a fit to the ellipsometric measurements provide additional information concerning the size distribution of sp^ 2 clusters, as reflected in the width of the π-π^* electronic transition. This width decreases as Si is added to the Si-AHC …