Deformation-induced microstructural modification is used for several advanced materials' processing methods such as friction-stir-based processing, welding, or additive manufacturing. In these processes, the mechanical-thermal coupling obscures a deep mechanistic understanding of the microstructural evolution of multi-phase metallic systems under extreme deformation, and the knowledge of how these microstructures influence mechanical properties is in its nascency. In this work we highlight the influence of high strain deformation on the microstructural hierarchy and mechanical properties of binary alloys such as Al-Si, Cu-X (X = Nb, Cr or Ni). Our studies show that deformation-induced grain refinement, multiscale fragmentation, and metastable solute saturated phases with distinctive defect structures lead to a significant increase in the flow stresses measured via micropillar compression. These results highlight that shear deformation during solid-phase processing can achieve persistently metastable microstructures with enhanced mechanical properties alloys with varying solute miscibility. The experimental insights obtained here are crucial for developing atomic-scale to mesoscale predictive models for microstructural evolution of alloys under high strain deformation.