The use of gold in medicine has a long history that dates back to ancient times. In modern medicine, gold compounds have been applied as anti-inflammatory agents for the treatment of rheumatoid arthritis. Recently, gold complexes have gained increasing attention in the design of metal-based anticancer chemotherapeutics. Gold(i) and gold(iii) ions are often unstable or reactive via redox reactions under physiological conditions. By judicious selection of coordination ligands, gold(i) and gold(iii) complexes that are stable under physiological conditions can be prepared and harnessed for anticancer applications. In this chapter, our current understanding on the anticancer properties of gold compounds and the approaches to identify their molecular targets and improve anticancer efficiency are reviewed.