Nanomaterials have garnered increasing interest recently as potential therapeutic drug-delivery vehicles. Among the existing nanomaterials are the pure carbon-based particles, such as fullerenes and nanotubes, various organic dendrimers, liposomes and other polymeric compounds. These vehicles have been decorated with a wide spectrum of target-reactive ligands, such as antibodies and peptides, which interact with cell-surface tumor antigens or vascular epitopes. Once targeted, these new nanomaterials can then deliver radioisotopes or isotope generators to the cancer cells. Here, we will review some of the more common nanomaterials under investigation and their current and future applications as drug-delivery scaffolds with particular emphasis on targeted cancer radiotherapy.