It is now well established that the processing of bulk solids through the application of severe plastic deformation (SPD) leads to exceptional grain refinement to the submicrometer or nanometer level. Extensive research over the last decade has demonstrated that SPD processing also produces unusual phase transformations and leads to the introduction of a range of nanostructural features, including nonequilibrium grain boundaries, deformation twins, dislocation substructures, vacancy agglomerates, and solute segregation and clustering. These many structural changes provide new opportunities for fine tuning the characteristics of SPD metals to attain major improvements in their physical, mechanical, chemical, and functional properties. This review provides a summary of some of these recent developments. Special emphasis is placed on the use of SPD processing in achieving increased electrical conductivity, superconductivity, and thermoelectricity, an improved hydrogen storage capability, materials for use in biomedical applications, and the fabrication of high-strength metal-matrix nanocomposites.