Both high tensile ductility and high strength are achieved in bulk multi-modal (Multi-Ni) and bimodal (Bi-Ni) nanostructured nickel, synthesized by cryomilling and subsequent quasi-isostatic forging processes. The relatively low tensile ductility of bulk nanostructured materials has been a major obstacle for their practical applications. This work provides a new approach for fabricating bulk nanostructured materials with both high ductility and strength.