Use of carbon materials is no longer limited to diamond jewelry or graphite pencils and lubricants. The last decade has witnessed an explosion of technological applications driven by the development of fabrication methods and the discovery of several new classes of pure carbon. Structural diversity exhibited by the carbon atoms, from local chemical order to long-range crystalline order, is key to understanding their physical and chemical properties and in future materials development. This article summarizes the use of Raman spectroscopy as a principal tool to investigate the vibrational dynamics of carbon materials and to provide indirect structural characterization of their short-, medium- and long-range order