Large‐scale ordered nanostructure arrays on substrates, including nanowires, nanotubes, nanodots, and nano‐holes, can be fabricated using template fabrication processes. The controllable structural parameters and properties of the ordered nanostructure arrays make them quite suitable to be used in many device‐related application areas. It is shown that large‐scale nanowire arrays are good candidates for the realization of a nano‐generator based on the piezoelectric effect of ZnO nanowires. The mechanism of a proposed high‐efficient nano‐generator based on an assembled nanowire/nanohole embedded structure shows high application potentials for biological and nanometer‐sized devices.