Electroformed copper layer with nanostructure is obtained using a subsequent mechanical treatment under the conditions of ultrasonic vibration according to the demand of high performance material in aeronautics. The microstructure of the electroformed copper layer is observed by optical microscope (OM), scanning electron microscope (SEM) and transmission electron microscope (TEM). The tensile strength is evaluated with a tensile tester. It is found that bulk crystal of electroformed copper’s surface layer is changed to nanocrystals (about 10 nm in size) after the ultrasonic-assisted mechanical treatment (UMT) but the whole monocrystalline structure still remains. The tensile strength exhibited by the new copper layer is two times better than the regular electroformed copper layer, while the fracture strain remains constant. In addition, the strengthening mechanism of UMT process is proved to be dislocation strengthening mechanism.