A comparative study of arF- and KrF-laser deposition of amorphous diamond-like carbon (DLC) films and relevant carbon plasmas has been performed. Spectroscopic ellipsometry and EELS analysis of the DLC films deposited on Si <100> and NaCl substrates were utilized to characterize the high quality arF- and KrF-laser deposited films (up to 84% of sp3 bonded carbon in 7 J/cm2 -ArF-laser DLC film). Gated ICCD imaging, luminescence and ion current probe diagnostics of the carbon plume have revealed quite different properties of carbon plasmas generated by arF- and KrF- lasers. KrF-laser (6.7 J/cm2) irradiation produces a less energetic carbon plasma containing larger amounts of C2 and probably larger clusters compared with arF-laser irradiation at the same energy fluence. We conclude that the more energetic and highly-atomized arF-laser carbon plasma results in the better diamond-like properties.