The radical polymerization of styrene and n-butyl acrylate is demonstrated to proceed under controlled conditions between 125 and 130 degrees C in the presence of either a 1,5-dimethyl-3-phenyl-6-oxoverdazyl radical or a 1,5-dimethyl-3-ethyl-6-oxoverdazyl radical producing polymers with polydispersity indices in the 1.2-1.3 range. While polymerizations initiated with benzoyl peroxide or 1,1-azobis(cyanocyclohexane) in the presence of verdazyl radical were unsuccessful, polymerizations initiated with a styrene/verdazyl unimolecular initiator proceeded in a living fashion, although quite slowly. An increase in polymerization rate was obtained with a 1,5-dimethyl-6-oxoverdazyl radical, producing higher yields of well-defined polymers. The livingness of the resulting styrene and n-butyl acrylate homopolymers is illustrated with chain extension reactions to make well-defined diblock copolymers. These results open a new front in the development of living-radical polymerization processes, and the ability to manipulate the verdazyl structure offers the opportunity to further control and modify this process.