Nanostructured or partially amorphous Al-and Zr-based alloys are attractive candidates for advanced high-strength lightweight materials. Such alloys can be prepared by quenching from the melt or by powder metallurgy using mechanical attrition techniques. This work focuses on mechanically attrited powders and their consolidation into bulk specimens. Selected examples of mechanical deformation behavior are presented, revealing that the properties can be tuned within a wide range of strength and ductility as a function of size and volume fraction of the different phases.