The lack of a comprehensive understanding of the role of heat treatments on microstructure and multiscale mechanical properties of powders and their interrelatedness with cold spray process parameters severely impedes the manufacturing of high-strength aluminum coatings. For the first time, this study develops customized heat treatment protocols for controlling microstructure homogenization and intermetallic precipitation in Al 6061 and Al 7075 powders for cold spray. Solution treatment at 505-545 °C, followed by precipitation hardening at 130-160 °C, enables controlled precipitation of hard intermetallic Mg2Si and MgZn2 phases in Al 6061 and Al 7075, respectively. Strengthening by these phases enhances powder nanohardness of Al 6061 and Al 7075 from 1.0 and 1.5 to 1.6 and 1.8 GPa, respectively. The cumulative response from multiple grains at the micrometer length scale carries the trend to improve microhardness to 131.2 and 177 HV. These characteristics of the precipitation-hardened powder encompass improvements of 13-60% above their pristine gas-atomized counterparts. Experimentally measured powder hardness was employed as input in a cold spray simulation tool to develop process maps for manufacturing high-quality coatings. The optimum temperature for deposition with 75-98% efficiencies was established to be 100-300 °C with helium and 500-600 °C with nitrogen and air. In this process window, the particle velocity and critical velocity range of the powders are 998 to 1237 ms−1 and 548 to 858 ms−1 for helium and 580 to 663 ms−1 and 400 to 594 ms−1 for air and nitrogen, respectively. [ABSTRACT FROM AUTHOR]