There is much current research into improving chemotherapy using approaches based on nanotechnology and polymer chemistry. In this review, the issues around approaches to improving chemotherapy using such constructs are briefly introduced, before focusing on an interesting class of globular polymers (dendrimers) as nanocarriers for chemotherapy drugs. The nature of association of the drug to the dendritic carrier is critical to the delivery of chemotherapeutics. So far, however, an examination of which of these two approaches is most ideally suited to the development of tumor delivery systems for chemotherapeutic drugs has been limited to a few isolated studies. Consequently, in this review we compare the known outcomes of the two broad drug association strategies to enable a rational conclusion to be drawn about the most likely successful strategies to employ in designing and developing dendrimer-based drug delivery systems.