We have deposited diamondlike carbon (DLC) films on a variety of substrates from 250° C and higher. The effects of deposition temperature on the properties of DLC films deposited by a conventional laser ablation technique are compared with that of a unique laser-plasma deposition scheme. The calculated values of neff, the effective number of valence electrons, suggest that, with the increase in the deposition temperature, the diamondlike component (sp3 bonds) remains invariant for the laser deposited samples, and increases for the laser-plasma deposited films. Raman measurements show that the Raman allowed ‘G’ band upshifts to ˜1600 cm−1 for both deposition schemes. However, the disorder induced 'D' band remains invariant at ˜1370 cm−2 for the laser ablated samples, and downshifts to ˜1350 cm−1 for the laser-plasma deposited samples. These results suggest a correlation between the diamondlike content (sp3 bonds) and the Raman shift of the ‘D’ band.