The electron-ion dynamics of hydroperoxyl radical in intense femtosecond laser pulses is studied by using time-dependent density functional theory combined with molecular dynamics approach. We calculate the optimized structure, the ionization energy, and the optical absorption strength. The results are in good agreement with experiments. The irradiation dynamics of HO2 including the ionization, the dipole moment, the bond lengths, the kinetic energies, and the level depletion is explored by varying the laser frequency. Computational results indicate that the excitation behaviors are distinct due to different frequencies. Furthermore, the angular dependence of the total ionization and the orbital ionization yields of HO2 are explored. The calculated result predicts a maximum around [Formula: see text] and [Formula: see text] for the total ionization and the angular dependence of the total ionization reflects the symmetry of the HOMO.