Nanocrystalline metals developed based on fine grain strengthening always have an excellent strength, but are accompanied by a drop in ductility. In the past 20 years, substantial efforts have been dedicated to design new microstructures and develop the corresponding processing technologies in order to solve this problem. In this article, the novel nanostructures designed for simultaneously achieving high strength and high ductility developed in recent years, including bimodal grain size distribution nanostructure, nanotwinned structure, hierarchical nanotwinned structure, gradient nanostructure, and supra-nano-dual-phase nanostructure, are reviewed. Based on a comprehensive understanding of the simultaneously strengthening and toughening mechanisms, the microstructures and corresponding processing techniques are mainly discussed, and the related prospects that may be emphasized in the future are proposed.