The infrared (IR) spectrum and vibrational predissociation of the proton-bound H2O+-Ar ionic complex are investigated within an ab initio and quantum dynamical study. For this purpose, a two-dimensional potential energy surface (2D PES) is determined as a function of the HO-H and OH-Ar coordinates. This PES is then employed in a wave-packet calculation to determine spectral properties of the system and to calculate the IR absorption spectrum. The vibrational energy levels and relative IR intensities agree well with the experimental spectrum reported earlier. On the other hand, the predissociation lifetimes in the nanosecond regime derived from the 2D PES are in disagreement with the experimental observations, indicating the importance of the neglected degrees of freedom for a correct description of the dynamics of the complex. (C) 2004 American Institute of Physics.