The chemistry of carbon nanotubes has become an area of intense research as chemical derivatization is the only means for modifying the properties of these highly interesting and technologically promising materials. Specifically, numerous researchers have focused on improving the solubility of carbon nanotubes through chemical grafting. To this end, significant recent effort has been devoted to the attachment of polymers to the nanotube surface, as macromolecules can be more effective in modifying nanotube solubility properties than small molecules. In addition, the use of functional polymers has enabled the preparation of polymer-nanotube composite materials that demonstrate a variety of interesting properties, such as responsiveness to environmental stimuli (solvent, temperature, pH), the ability to complex metal ions, and photoinduced electron transport. A variety of different techniques have now been developed for the functionalization of carbon nanotubes with polymers, including "grafting to", "grafting from", and supramolecular interactions. This review will focus on recent developments in the use of living radical polymerization methods for the functionalization of carbon nanotubes with well-defined polymers.