Providing materials with an inner architecture that improves their mechanical and physical properties is a potent approach to materials design. Herein, the possibilities of such architecturing by means of severe plastic deformation (SPD) are discussed. Compositional and structural patterns caused by SPD processing can potentially improve the mechanical characteristics and physical properties of exemplary materials considered. The message to convey is that SPD opens up new opportunities with regard to producing materials with a multiscale structure. This can be achieved by virtue of the following effects associated with SPD: extreme grain refinement, whose level is governed by strain distribution; controlled self-organization of the structure of multiphase materials; and anomalously fast mass transfer, which leads to the formation of new phases and various "reaction-diffusion" patterns. Furthermore, combining SPD with conventional metal forming, differential heat treatment, or 3D printing offers additional possibilities, which are considered in this article.