One of the most promising applications of nanotechnology is that of drug delivery, and in particular the targeted delivery of drugs using nanotubes. Functionalized nanotubes might be able to target specific cells, become ingested, and then release their contents in response to a chemical trigger. This will have significant implications for the future treatment of patients, particularly those suffering from cancer, for whom presently the nonspecific nature of chemotherapy often kills healthy normal cells. Research to date has largely been through experiments investigating toxicity, biocompatibility, solubility, functionalization, and cellular uptake. More recently, the loading and unloading of molecular cargo has gained momentum from both experimental and theoretical investigations. This Review focuses on the loading and unloading of molecular cargo and highlights recent theoretical investigations, which to date have received very little attention in the review literature. The development of nanotube drug-delivery capsules is of vital concern for the improvement of medical treatment, and mathematical modeling tends to facilitate such development and provides a quicker route to applications of the technology. This Review highlights the latest progress in terms of theoretical investigations and provides a focus for the development of the next generation of medical therapeutics.