A brief overview will be given of the remarkable structure and properties of carbon nanotubes and how surface interactions are used for some of these studies. Carbon nanotubes are tiny structures of molecular dimensions in the form of hollow cylinders with about 20 carbon atoms around the circumference of the cylinders and microns in length. The unique electronic properties of carbon nanotubes are that they can be either semiconducting or metallic depending only on their geometry. From this, stem other remarkable and unique properties of their vibrational spectra, allowing us a means to distinguish metallic from semiconducting nanotubes in samples containing both. Interactions of the nanotubes with nanostructured metallic substrates have provided a powerful tool to gain a fundamental understanding about why the Raman spectra of metallic nanotubes are different from those for semiconducting nanotubes. Though less than a decade since their discovery, carbon nanotubes are already finding practical applications based on their unique properties.