The picosecond laser irradiation of diamond-like carbon (DLC) film on the silicon wasinvestigated. The DLC films were irradiated by Nd:YVO4 laser with the infrared (1064 nm, fluency 1.02 J/cm2) and ultraviolet (355 nm, fluency 0.79 J/cm2) wavelengths with 1, 10, and 100 pulse numbers per spot. The energy dispersive X-ray spectroscopy and microRaman spectroscopy measurements indicated that the full ablation area of the DLC was narrower than laser beam radius of the 1064 nm wavelength with 10 and 100 pulses. The increase of the oxygen concentration was obtained near the ablation areas after irradiation with the first harmonic. The microRaman and SEM measurements demonstrated that the DLC film was fully ablated in the laser spot when the third harmonic was used. The formation of silicon carbide (SiC) in the center of the irradiated spot was found after 100 pulses.