Copper (Cu) is an essential micronutrient involved in a variety of fundamental biological processes. Recently, disorder of Cu homeostasis can be observed in many malignancies. Elevated Cu levels in serum and tissue are correlated with cancer progression. Hence, targeting Cu has emerged as a novel strategy in cancer treatment. This review provides an overview of physiological Cu metabolism and its homeostasis, followed by a discussion of the dysregulation of Cu homeostasis in cancer and the effects of Cu on cancer progression. Finally, recent therapeutic advances using Cu coordination complexes as anticancer agents, as well as the mechanisms of their anti‐cancer action are discussed. This review contributes full comprehension to the role of Cu in cancer and demonstrates the broad application prospect of Cu coordination compounds as potential therapeutic agents.