Pure copper (Cu) having bimodal 'harmonic structure' (HS) was fabricated by a technique based on severe plastic deformation of powders, which involved tailored mechanical milling and spark plasma sintering. The harmonic-structured Cu demonstrates a unique combination of high strength and large elongation superior to its homogeneous as well as bimodal heterogeneous counterparts. Specific features of harmonic structure, i.e. continuous network of ultra-fine grained (UFG) regions encompassing coarse-grained areas, lead to the extension of uniform elongation. The optimum combination of properties in pure Cu is found to be in the harmonic-structured material having 40 % UFG fraction.