The use of cold spray deposition, coupled with diffusion-driven thermal postprocessing, is considered herein as a surface modification process such that near-surface microstructural, micromechanical, and microchemical property improvements can be procured for cost-effective and common aluminum alloy castings. Since the present work was an exploratory investigation into the realm of cold spray induced, high-pressure diecast aluminum subsurface property development and evolution, as well as surface modification, one significant aim was to formalize a set of fundamental observations for continued consideration of such an approach to achieving premium aluminum alloy properties from cost-effective alternatives. Nickel, copper, and titanium cold spray modified near-surface regions of the cost-effective high-pressure diecast A365 system was considered. Near-surface, subsurface, and surface evolution was documented across each of the three pure metal coatings. The analysis was continued across two postprocessing coating-substrate atomic diffusion inspired heat-treated conditions as well. Using energy-dispersive X-ray spectroscopy, field-emission scanning electron microscopy, optical microscopy, and various insights gleaned from an original contextualization of the relevant cold spray literature, noteworthy results were recorded and discussed herein. When copper feedstock was employed alongside thermal postprocessing, diverse surface-based intermetallic compounds formed alongside exotic diffusion zones and severely oxidized regions, thus eliminating thermally activated copper cold-sprayed consolidations from future work too. However, both nickel and titanium cold spray surface modification processing demonstrated potential and promise if correct processing stages were performed directly and chronologically. Consequently, a platform is presented for further research on cold sprayed surface microstructural and property modification of cost-effective alloyed aluminum castings.