Magnetic storage discs overcoated under different conditions with sputtered carbon in the presence of hydrogen were analyzed for hydrogen/carbon content by nuclear reaction analysis (NRH:C), for thickness and optical absorption by ellipsometry, for carbon structure (D and G bands) by fast micro-Raman spectrophotometry, and for C-H bonds by polarized reflection Fourier transform infrared (FTIR) spectrophotometry. CSS wear performances were compared with the analytical data. It was observed that wear performance improved with increases of D and G Raman band frequencies, DIG Raman intensity ratios, integrated CH2band intensity in the FTIR spectrum, and optical absorptivity, but with decreases of NRAH:C, up to a limiting value. A structural model is proposed to account for the observations.