Morphologically controllable copper sulfide (CuS) nanoneedle, nanowall, and nanosheet networks on copper substrates have been fabricated by a simple, facile, and fast method based on low-temperature chemical vapor deposition through simply adjusting the reaction conditions such as the temperature and flow rate of argon gas. The compositional and structural analyses indicated that all the obtained nano-networks were single-crystalline. And their growths were possibly controlled by a solid–liquid–solid mechanism. The photocatalytic activities of the different shaped CuS nanostructures have been evaluated by their photodegradation on rhodamine B and methylene blue in aqueous phase, which revealed that in both cases the CuS nanoneedles nano-network exhibited better performance than the other two nanostructures.