Up to now, the polypharmacology of diterpene alkaloids isolated from Aconitum and Delphinium sp. has been extensively studied. From 1998 to 2014, more than 400 new diterpene alkaloids were isolated from Nature. Pharmacological researches have indicated that many diterpenoid alkaloids are the main bioactive components which have arrhythmogenic, local anesthetic, antiarrhythmic, curariform, analgesic, hypotensive, anti-inflammatory, anti-microbial, anti-tumor, spasmolytic, neurotropic and psychotropic activities. In the present review, the antiarrhythmic, analgesic and anti-inflammatory activities of diterpene alkaloids as well as the pharmacological mechanisms were summarized. Moreover, their Structure-Activity Relationship was also analyzed.