Several common elementary methods of computing molecular properties, prerequisite to molecular dynamics studies, are tested for their validity for CS2+. Judged sufficiently accurate, these methods are then used to aid in investigating the collisionally activated dissociation of CS2+ upon impact with xenon. Rice-Ramsperger-Kassel-Marcus (RRKM) unimolecular decay rate calculations are presented and compared to experimental studies employing collisional activation. RRKM theory is shown to reproduce the experimental results for collision energies near threshold. When corrected for vibrational anharmonicity, the RRKM calculation shows agreement with the experimental results over a slightly wider range of energies. A discussion is given on the applicability of the "adiabatic criteria" to describing electronic excitations in the collisional activation process. This model is shown to provide a better description of the activation process than direct vertical excitation.