Licorice is a traditional medicine commonly used in China and many other countries. Over the last 50 years, the structure and pharmacological effects of coumarin compounds in licorice have been investigated. However, a comprehensive review of the literature summarizing current trends is currently lacking. Thus, the aim of the present review is to provide an up-to-date summary of the scientific literature regarding the pharmacological effects of coumarin compounds in licorice, thereby laying the foundation for further research and optimal utilization of licorice. We retrieved 111 articles on the coumarin components of licorice and their potential pharmacological effects, based on titles, keywords, and abstracts from databases (including PubMed and Web of Science). Glycycoumarin, isoglycycoumarin, licoarylcoumarin, licopyranocoumarin, glycyrin, isotrifoliol, glycyrol, and glycyrurol have been investigated for their anticancer, hepatoprotective, antispasmodic, immunosuppressive, anti-inflammatory, and antibacterial properties, and use as therapeutic agents in metabolic syndrome, thereby demonstrating their potential for clinical applications. Future research should further explore the pharmacological mechanisms of action of coumarin compounds, including their antibacterial activities. Investigations into the pharmacological activities of different glycycoumarin isomers might open new research frontiers.