The tensile strength of nanostructured Cu obtained by electrodeposition and Surface Mechanical Attrition Treatment (SMAT) was studied. Cu after electrodeposition had been first studied. Electrodeposited Cu had the well-known reduction on the grain size and as well as the improvement on the strength compared with the bulk hard copper. After SMAT, although the ductility had dropped, the yield strength is further enhanced up to 50% (350MPa) to obtain a stronger material. Since the parameters of the electrodeposition affects the properties of the materials obtained, rooms for improvement could be expected, for example, increasing the duration of the electrodeposition may increase the ductility significantly, in the later stage of this study, experimental results proved this saying. The present study demonstrates the potential process for developing a novel surface nanostructured material with electrodeposited Copper with SMAT for engineering applications. Copyright © 2007 by ASME.