Volatile oil (VO) is the main chemical component of common plants in Chrysanthemum genus, and it possesses several beneficial pharmacological properties, including bacteriostatic, antioxidant, anti-tumor, anti-inflammatory, antipyretic, analgesic, anti-osteoporotic, antihypertensive, sedative, and hypnotic effects. To date, research on the effective components of Chrysanthemum extract has mainly focused on flavonoids, whereas limited data are available on the chemical constituents and underlying mechanisms of action of the VO components. In this review, the pharmacological activities and mechanisms of VO are comprehensively reviewed with the aim of providing a foundation for further development for medicinal, aromatherapy, and diet therapy applications.