To date, many potent metal-based anticancer drugs have been developed and many drug delivery systems have been exploited to improve the targeting and decrease the side effects of anticancer drugs. Human serum albumin (HSA) binding contributes significantly to the discovery of new drug candidates because binding of drugs to HSA strongly influences their pharmacokinetic behaviour. Moreover, HSA is widely used in the clinical setting as a drug delivery system due to its potential for improving targeting while decreasing the side effects of drugs. This review not only provides a brief outline of the properties of HSA carriers but also provides an overview of the binding and anticancer characteristics of platinum-/ruthenium-based anticancer drugs to HSA that may guide the rational designing and development of metal-based drugs and HSA-based carriers for clinical applications.