Generation of multiply charged ions and molecular ions have been investigated using simultaneous irradiation of high intensity and ultrashort pulse of Ti:sapphire laser and fourth harmonics of Q-switched nanosecond pulse of Nd:YAG laser on carbon targets [Morimoto et al., in: Proceedings of the 13th International Conference on High-Power Particles Beams (BEAMS2000),Vol. PB-89, Nagaoka, 2000, p. 359; Toyoda et al., in: Proceedings of the 8th International Symposium on Gas Flow and Chemical Lasers and High-Power Laser Conference (GCL-HPL2000), Vol. P1.60,2000, p. 101]. The ion current waveforms have been analyzed by means of time-of-flight (tof) mass measurement. Simultaneous irradiation of high intensity and ultrashort pulse of Ti:sapphire laser and fourth harmonics of Q-switched nanosecond pulse of Nd:YAG laser on carbon targets was found to generate molecular ions of carbon. (C) 2002 Published by Elsevier Science B.V.