The research in this article explores the response of semicrystalline isotactic polypropylene to gamma radiation in air, and relates the morphological changes of the polymer to corresponding changes in mechanical properties. The effect of the initial morphology of the polymer on its response to irradiation is considered using infrared spectroscopy (FTIR), small- and wide-angle X-ray scattering, dynamic mechanical thermal analysis (DMTA), and mechanical testing. The extent of chain scission and crosslinking is dependent on the dose but not the initial starting morphology. These chemical changes cause the crystallinity to increase slightly, and the glass transition temperature to rise by a few degrees in all samples, but the overall morphology is only subtly changed. In contrast, a major deterioration in mechanical properties is caused. The effects of the irradiation observed under these conditions are similar in each material and the ultimate properties determined by the properties seen in the original material.