Refinement of microstructure from ordinary coarsegrained (CG; grain size d ! 10 mm) down to ultrafine-grained (UFG; grain size d 1 mm), and even further to nano-scale, is a well-proven approach for the strengthening of metallic materials. [1][2][3] However, the downside of bulk UFG metals is their rather poor ductility resulting from very limited capacity for dislocation storage and therefore early strain localization during mechanical loading. [2][3][4][5] Since both strength and ductility are important characteristics for the majority of structural applications, various strategies have been suggested to improve the ductility of bulk UFG and nano-structured metals and alloys. [5,6] Among these strategies, fabricating structures with rather wide, gradient or, better, bimodal grain size distributions appear to be very efficient for the enhancement of ductility at a little compromise in strength. [7,8] In such structures, the ultrafine-and nano-scale grains provide the high strength, while the coarser grains store dislocations, therefore, enhancing the ductility characteristics. [3][4][5] Recently, a substantial number of processing routes allowing the fabrication of metallic materials with bimodal grain size distributions have been developed. [8][9][10][11] These routes are based on severe plastic deformation (SPD) [10] and other thermo-mechanical processing techniques [8,9] as well as on powder metallurgy approach. The latter involves mechanical milling (MM) of metal powders, mixing of the MMed and the initial powders (IP), and finally consolidating the mixture. [11] Such processing routes, although effective in the control of UFG/CG fraction ratios, provide very limited control over the spatial topological distribution of the coarse and the fine grains. Therefore, these limited-control microstructures deliver only a limited control over properties.In order to improve the control over the microstructural characteristics, and thus properties, Ameyama and co-workers [12][13][14] recently proposed a novel approach based on the powder metallurgy route. Its peculiar features are: (i) the MM processing is optimized to induce heterogeneous structure in powder particles having CG and nano/UFG structures in their core and periphery, respectively; and (ii) the consolidation is optimized to preserve the heterogeneity. Bulk materials fabricated in this way have bimodal structure with a specific regular spatial distribution of nano/UFG and CG regions. Namely, CG structure is enclosed in a three-dimensional continuously connected network of nano/UFG structure. Therefore, we call them "harmonic structured" materials. Further details about the fabrication route, the "harmonic structure" (HS) design concept, and the benefits of them can be found elsewhere. [12][13][14] Although both the ordinary limited-control bimodal structures and the HSs exhibit a very appealing combination of strength and ductility, the variation of the mechanical properties can be quite large. [6] It is envisaged that the large variation of the mechanical ...