The important pharmacological activities and structural complexity of diterpenoid alkaloids have long stimulated strong scientific interest; some of these naturally abundant compounds have been reported to be highly promising for treating cancer. From 2008 to 2018, the cytotoxicity activities of more than 250 diterpenoid alkaloids were tested against several cancer cell lines. This review focuses on the progress of diterpenoid alkaloids with different structures derived from Ranunculaceae plants and some of their derivatives with potential anticancer activities. Then, we discuss the application prospects and development of active diterpenoid alkaloids.