This paper provides an overview of the role of nanomaterials in emerging nanoelectronic devices. As semiconductor devices are scaled to smaller and smaller sizes within the nanoregime, a variety of technological and economic problems arise, the rules of classical physics give way to quantum mechanics, and the term molecular-scale ultimately becomes as or more accurate than nanoscale. At this point, the size scaling that has successfully taken device features from the microscale to the nanoscale can no longer be continued, and alternative processing technologies, materials, and device structures are required. In this regime, nanostructured materials, including quantum dots, semiconductor nanowires, and carbon nanotubes, become essential to continued miniaturization and performance enhancement.