Due to their potential applications, ranging from nanoscale electronic devices to tools for biomedical applications, onedimensional semiconductor nanostructures, such as nanowires and nanobelts, offer a high degree of interest for furthering the current state of nanotechnology research and development. Nanorods, 1 nanowires, 2 nanotubes, 3 and nanobelts 4 of various materials have been successfully synthesized, and they demonstrate novel luminescent, electronic, optical, and mechanical properties.ZnS is a direct wide band gap (3.91 eV) compound semiconductor that has a high index of refraction and a high transmittance in the visible range and is one of the most important materials in photonics research. 5 As a one-dimensional nanostructure, ZnS has been synthesized as nanowires, nanobelts, and nanocombs, but these nanostructures are randomly distributed on the surface of the substrate. 6,7 For applications in photonics, it is needed to create ZnS nanostructures that are highly aligned and ordered, but this type of structure has not been realized experimentally. In this paper, we report a novel approach for growing aligned and orientationordered ZnS nanowires. Our method relies on a buffer layer of CdSe grown on a Si(111) substrate, on which ZnS nanowires are grown. The growth process of the nanowire bundles is presented. The technique demonstrated could be an effective pathway for growing patterned, aligned, size-controlled, and orientation-ordered ZnS nanowires.The orientation-ordered ZnS nanowire bundles were synthesized through a two-step thermal evaporation process in a horizontal tube furnace. Commercially available CdSe powder (Alfa Aesar, 99.995% purity, metal basis) was placed in the center of a single-zone tube furnace (Thermolyne 79300). A vacuum was pulled into the tube for several hours to purge oxygen from the chamber. After evacuation to less than 2 × 10 -2 Torr, the temperature in the center of the tube was elevated to 750°C at a rate of 30°/min. A nitrogen (N 2 ) gas flow was introduced into the system at a rate of 50 sccm. The gas acted as a carrier for transporting the sublimated vapor to cooler regions within the tube furnace for deposition. The pressure was maintained at 300 mbar. The silicon substrates reached a temperature of about 575°C. After 1 h, the furnace was allowed to cool. Then, the source material of CdSe powder was replaced by commercially available ZnS powder (Alfa Aesar, 99.99% purity, metal basis). The temperature in the center of the tube was elevated to 1050°C. Again, a nitrogen gas flow was introduced at 50 sccm, and the pressure was maintained at 300 mbar. The silicon substrates reached a temperature of about 750°C. The system was held in this condition for a period of 60 min. Single-crystal silicon substrates were used for synthesizing the nanostructures. These substrates were placed downstream from the source material to collect the deposited nanostructures.The sample was analyzed on a scanning electron microscope (SEM). The deposited material has an extremely high yie...