Additive manufacturing is a rapidly growing industry with numerous technologies to suit a variety of applications. However, each application has its own inherent flaws and niches. Aluminum alloys are difficult for the more popular fusion-based additive manufacturing techniques due to the intense thermal gradients generating distortion and selective vaporization of alloying elements. To subjugate some of the issues, the solid-state Additive Friction Stir-Deposition (AFS-D) method was proposed to produce high quality, defect free aluminum deposits. This work investigates the process-structure-property relationships of two popular commercial aluminum alloys employed extensively by consumer, transportation, and defense industries. The first work on process-deformation characteristics of AA6061 were evaluated by producing microhardness profiles taken from the cross-section of builds to produce relationships between mechanical characteristics and machine parameters. Resulting average hardness values were plotted against the processing window and used to determine comparative samples for microstructural analysis. Electron backscatter diffraction and transmission electron microscopy was conducted to characterize the microstructural evolution of depositions. This study provides a succinct, multiscale characterization of as-deposited AFS-D AA6061 to expound the effect of the high-shear solid-state AM process. The subsequent investigation on AA6061 is the first investigation of the process-structure-property relationships of AFS-D in an overlapping, parallel raster deposit. In particular, the deposit produced in this work explores the influence of severe plastic deformation on the as-deposited microstructure and tensile response of material that overlaps in parallel layers at the outer edge of the tool. This study sought to determine the viability of producing large scale structural components larger than the track-width of the AFS-D tool. The final study quantifies the microstructural evolution and consequential tensile response of AA5083. A brief examination of the effect of AFS-D processing parameters was undertaken to determine preferential processing conditions for a larger, free-standing AA5083 structure. Optical and scanning electron microscopy evaluate the microstructural evolution of particles and grain morphology. Tensile properties were evaluated in the longitudinal and vertical build directions, and subsequent fractography discovered the influence of lubrication on the variable mechanical response.