The harmonic structure has a heterogeneous microstructure consisting of bimodal grain size together with a controlled and specific topological distribution of fine and coarse grains. In other words, the harmonic structure is heterogeneous on micro- but homogeneous on macro-scales. In the present work, the harmonic structure design has been applied to pure-Ti, Ni, Cu, Fe, Ti-6Al-4V alloy and SUS304L stainless steel via a powder metallurgy route consisting of controlled severe plastic deformation of the corresponding powder via mechanical milling or high pressure gas milling, and subsequent consolidation by SPS. At a macro-scale, the harmonic structure materials exhibited significantly better combination of strength and ductility, under quasi-static loadings, as compared to their homogeneous microstructure counterparts. This behavior was essentially related to the ability of the harmonic structure to promote the uniform distribution of strain during plastic deformation, leading to improved mechanical properties by avoiding or delaying localized plastic instability.