Two new C18-diterpenoid alkaloids, anthriscifoltine A (1) and anthriscifoltine B (2), along with three known diterpenoid alkaloids, deoxydelcorine (3), anthriscifolcine A (4) and anthriscifolcine G (5), were isolated from the whole herbs of Delphinium anthriscifolium var. majus. Their structures were elucidated by spectroscopic methods, including 1D, 2D NMR, and HR-ESI-MS.