Abstract: Human serum albumin (HSA) is a multi-functional protein, which is able to bind and transport a variety of endogenous and exogenous compounds. HSA can be used as a drug carrier in the targeted delivery of cancer drug therapy. To bind to HSA, a large variety of strategies has been developed through adding functional chemical groups to the drug molecule, thus changing the pharmacokinetics, increasing the circulation time of the drug in the blood without significantly affecting its biological activity. This strategy can increase the concentration and prolong the time of radiotherapeutic drugs at the tumor site and improve the effect of radionuclide targeted therapy. Drugs binding to HSA has been exploited to evaluate cardiac function, vascular permeability, and lymphography. In this review article, the recent developments of various ligands binding to HSA in the diagnosis and treatment of nuclear medicine are reviewed.