Nanostructured (NS) materials, with average grain sizes typically below 100 nm, are of considerable interest in both scientific and industrial communities. From a scientific viewpoint, interest stems from uncovering novel plastic deformation mechanisms, such as inverse Hall-Petch effect [1,2] and ductile-to-brittle transition. [3,4] From a technological standpoint, it is argued that NS materials may have distinctive mechanical properties in comparison to their coarse-grained (CG) counterparts, resulting in attractive application prospects. In fact, NS materials often exhibit ultrahigh strength and hardness, but at the expense of a much reduced ductility. For example, tensile tests [5][6][7][8][9] on pure NS Cu have shown the yield strength in excess of 400 MPa, which is six times higher than that of CG Cu. However, tensile elongation obtained in these tests is well below 5 %, and it decreases with decreasing the grain size. The disappointingly low ductility can be attributed to the artifacts from processing, the mechanical instability with little or no strain hardening capacity, and low toughness and resistance to crack initiation and propagation. [10] Recently, extensive research has focused on the ductility problem in NS materials and there are indeed examples of optimized strength and ductility in a limited number of cases. Some examples documented their high ductility to the development of bimodal grain size distributions, [11] twin densities [12,13] and strain rate sensitivity. [14][15][16] In other examples, [17][18][19] however, the reasons for enhanced ductility are not clearly defined.In this communication, we fabricated a pure NS Cu through a direct-current eletrodeposition technique. Tensile tests on this NS Cu clearly demonstrated an improved combination of strength and ductility at different strain rates. The mechanism contributing to the high ductility was discussed by the observation on its microstructures as well as the fracture surfaces.The main impurities contents (mass ppm) of the as-deposited NS Cu are listed in Table 1. A relative high content of Pb is measured to be related with the anode material. By X-ray diffraction (XRD) analysis on {111} and {222} peaks with Williamson-Hall integral breadth method, the NS Cu is characterized by an average grain size of ∼ 34 nm and a microstrain of ∼ 0.21 %. Figure 1 shows the transmission electron microscope (TEM) bright-field and corresponding dark-field images of the NS Cu. The grains are mostly equiaxed and have random orientations. Growth twins and dislocations can be found inside some grains. The grain boundaries show no evidence of porosities or contaminations. Many grain boundaries in bright-field images are poorly defined, and they can only be distinguished by dark-field observations. From a statistical analysis of ∼ 400 grains measured from dark-field images, an average grain size of ∼ 90 nm with a lognormal distribution from 30 to 200 nm can be obtained. The main reason for the smaller grain size determined by XRD is that dipoles affect the pe...