Advanced structural materials are required to show both high strength and large ductility/toughness, but we have not yet acquired the guiding principle for that. The bulk nanostructured metals are polycrystalline metallic materials having bulky dimensions and average grain sizes smaller than 1 μm. Bulk nanostructured metals show very high strength compared with that of the coarse-grained counterparts, but usually exhibit limited tensile ductility, especially small uniform elongation below a few %, due to the early plastic instability. On the other hand, we have recently found that particular bulk nanostructured metals can manage high strength and large tensile ductility. In such bulk nanostructured metals, unusual deformation modes different from normal dislocation slips were unexpectedly activated. Unusual <c+a> dislocations, deformation twins with nano-scale thickness, and deformation-induced martensite nucleated from grain boundaries in the bulk nanostructured Mg alloy, high-Mn austenitic steel, and Ni-C metastable austenitic steel, respectively. Those unexpected deformation modes enhanced strain hardening of the materials, leading to high strength and large tensile ductility. It was considered that the nucleation of such unusual deformation modes was attributed to the scarcity of dislocations and dislocation sources in each recrystallized ultrafine grain, which also induced discontinuous yielding with clear yield drop universally recognized in bulk nanostructured metals having recrystallized structures. For discussing the nucleation of different deformation modes in atomistic scales, the new concept of plaston which considered local excitation of atoms under singular dynamic fields was proposed. Based on the findings in bulk nanostructured metals and the concept of plaston, we proposed a strategy for overcoming the strength-ductility trade-off in structural metallic materials. Sequential nucleation of different deformation modes would regenerate the strain-hardening ability of the material, leading to high strength and large tensile ductility. The strategy could be a guiding principle for realizing advanced structural materials that manage both high strength and large tensile ductility.