Diamond-like carbon (DLC) thin films were prepared by laser ablation deposition. The deposition process was carried out in a vacuum chamber at a base pressure of about 10−5 mbar using the focused beam from either an Nd:YAG laser or an XeCl excimer laser and a pyrolytic graphite target. The peak power density of the laser beam was about 108 W/cm2, and 1010 W/cm2. respectively. The effect of varying power density of the laser beam also was examined. The films were deposited on fused silica and silicon single crystal substrates between room temperature and 600 °C with and without hydrogen addition. The properties of the films were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), micro-Raman and Fourier transform infrared (FTIR) spectrometry, electrical conductivity and optical measurements. The best films were insulating (σ<10−6 Ω−1 cm−1), hard, partly transparent (optical gap 1.3 − 2.2 eV) and smooth without any particulates on the surface.