The concept of grain boundary (GB) engineering of ultrafine-grained (UFG) metals and alloys is developed for enhancement of their properties by tailoring different GBs (low-angle and high-angle ones, special and random, or equilibrium and nonequilibrium) and formation of GB segregations and precipitations by severe plastic deformation (SPD) processing. In this article, using this approach and varying regimes and routes of SPD processing, we show for several light alloys (Al and Ti) the ability to produce UFG materials with different GBs, and this can have a dramatic effect on the mechanical behavior of the processed materials. This article demonstrates also several new examples of attaining superior strength and ductility as well as enhanced superplasticity at low temperatures and high strain rates in various UFG metals and alloys.