Thin carbon films were synthesized by Pulsed Laser Deposition in vacuum or 0.5, 1, 10 mbar CH4 atmospheres on quartz and Si (100) substrates. The films had a very good compatibility with the Si (100) substrate, remaining adherent irrespective of the deposition temperature. For substrate temperatures below 200 °C, the films were not adherent to quartz, delaminating and forming flakes. At 200 °C, the films became adherent to quartz, but the bonding strength had values 40% lower compared to films synthesized on Si (100). The mismatch of the CTE was the most plausible cause for the layers incompatibility with the substrates. By introducing a buffer gradient layer with varying composition between substrate and films the bonding strength was increased by around 60%. The buffer had no effect on the bonding strength between Si (100) and the carbon films.