Hydrogen-free diamond-like carbon ͑DLC͒ films have been deposited with a 100 fs ͑FWHM͒ Ti:sapphire laser beam at intensities I in the 10 14-10 15 W/cm 2 range. The films were studied with scanning probe microscopy, variable angle spectroscopic ellipsometry, Raman spectroscopy, and electron energy loss spectroscopy. DLC films with good scratch resistance, excellent chemical inertness, and high optical transparency in the visible and near infrared range were deposited at room temperature. As the laser intensity was increased from 3ϫ10 14 to 6ϫ10 15 W/cm 2 , the films showed an increased surface particle density, a decreased optical transparency (85%˜60%), and Tauc band gap (1.4˜0.8 eV), as well as a lower sp 3 content (60%˜50%). The time-of-flight spectra recorded from the laser plume exhibited a double-peak distribution, with a high energy suprathermal ion peak preceding a slower thermal component. The most probable ion kinetic energy showed an I 0.55 dependence, increasing from 300 to 2000 eV, when the laser intensity was varied from 3ϫ10 14 to 6ϫ10 15 W/cm 2 , while the kinetic energy of suprathermal ions increased from 3 to over 20 keV and showed an I 0.33 dependence. These high energy ions are believed to have originated from an electrostatic acceleration field established by suprathermal electrons which were formed by resonant absorption of the intense laser beams.