Different nanoscaled hierarchical CuS superstructures, such as tree-like superstructures, nanowires, and nanowebs, have been prepared by a novel "ion-tailoring" method with clear advantages over the traditional complex approaches for the production of ID superstructured nanomaterials. Electron microscopy, X-ray diffraction, and optical spectroscopy were used to characterize the products. This novel designed strategy may be used for the preparation of other sulfide nanocrystalline superstructures.