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This monograph is a study of optimal control applied to cancer chemotherapy, the treatment of cancer using drugs that kill cancer cells. The aim is to determine whether current methods for the administration of chemotherapy are optimal, and if alternative regimens should be considered. The research utilizes the mathematical theory of optimal control, an active research area for many mathematicians, scientists and engineers. It is of multidisciplinary nature, having been applied to areas ranging from engineering to biomedicine. The aim in optimal control is to achieve a given objective at minimum cost. A set of differential equations is used to describe the evolution in time of the process being modelled, and constraints limit the policies that can be used to attain the objective. In this monograph, mathematical models are used to construct optimal drug schedules. These are treatment guidelines specifying which drug to deliver, when, and at what dose. Many current drug schedules have been derived empirically, based upon "rules of thumb". The monograph has been structured so that most of the high-level mathematics is introduced in a special appendix. In this way, a scientist can skip the more subtle aspects of the theory and still understand the biomedical applications that follow. However, the text is self-contained so that a deeper understanding of the mathematics of optimal control can be gained from the mathematical appendix.