This computational study of line‐broadening effects is based on an accurate, analytical representation of the intermonomer potential energy surface (PES) of the CO2•Ar van der Waals (vdW) complex. The PES is employed to compute collisional broadening coefficients for rovibrational lines of CO2 perturbed by Ar. The semiclassical computations are performed within the modified Robert–Bonamy approach, including real and imaginary terms, and the exact trajectory model. The lines investigated are in the 10001←00011, 01101←00001, 00011←00001, and 00031←00001 vibrational bands and the computations are repeated at multiple temperatures. The computed results are in good agreement with the available experimental values, validating both the intermonomer PES developed and the methodology used. For lines in the 01101←00001 band of CO2 temperature‐dependent Ar‐broadening coefficients are reported for the first time. The parameters presented should prove useful, among other applications, for the accurate experimental determination of CO2 and Ar abundances in planetary atmospheres.