Diamond-like carbon (DLC) films were deposited by pulsed laser ablation (PLA) on Si (100) and Ti-6Al-4V alloy substrates at four different temperatures. The bonding characteristics of the films were studied by X-ray photoelectron (XPS) and Raman spectroscopy techniques. The ratio of tetrahedral to trigonally coordinated carbon atoms was estimated by XPS successfully. The fraction of tetrahedrally bonded atoms in the films deposited on Si at room temperature was estimated to be ~63 at.% which decreased to ~33 at.% as the substrate temperature increased to 400 o C. The Raman spectroscopy results of these specimens agree qualitatively with these observations. Also, using Raman spectroscopy, the residual compressive stress was also estimated in fully adherent films on Si substrate to be ~3 GPa with reference to the value of stress present in a free-standing peeled off film from the Ti-alloy substrate. This value is consistent with the residual stresses estimated in the earlier results. The abrasive wear rates have been correlated during the initial stages of the well adhered films with the sp 3 /sp 2 ratios. The importance of suitable dopants and the interfacial interlayers in reducing internal compressive stresses in these films is discussed.