We theoretically investigated the stability of highly charged fullerene cations produced with an ultrashort intense near-infrared (IR) laser pulse (light intensity I∼ 5 × 1014 W/cm2 and wavelength λ ∼ 1800 nm). The effects of nonlinear interactions with near-IR pulses are taken into account by combining an ab initio molecular dynamics method with an time-dependent adiabatic state approach. The results indicate that large-amplitude vibration with energy of > 10 eV is induced by impulsive Raman excitation in the delocalized hg(1)-like mode of C602+. The field-induced large-amplitude vibration of the hg(1) mode persists for a rather long period. In conclusion, C 60 and its cations created upon ionization are extremely robust against field-induced structural deformation. We found that the acquired vibrational energy is maximized at Tp ∼ Tvib/2, where Tp is the pulse length and Tvib is the vibrational period of the hg(1) mode. We confirmed that the vibrational energy deposited in C60 can be controlled by a pulse train, i.e., by changing the intervals between pulses. Vibrational mode selectivity is also achieved by adjusting the pulse intervals.