Three new C-19-diterpenoid alkaloids, brevicalcarines A similar to C (1 similar to 3), together with seven known compounds (4 similar to 10), were isolated from the roots of A. brevicalcaratum (Finet et Gagnep.) Diels. Their structures were determined by HR-ESI-MS (high resolution electrospray ionization mass spectroscopy), IR (Infrared absorption spectroscopy), 1D NMR (One-dimensional nuclear magnetic resonance), 2D NMR (Two-dimensional nuclear magnetic resonance) and X-ray crystallographic analysis. Brevicalcarine A (1) was a new diterpenoid alkaloid with vaginatunine A fragment at C-18, while brevicalcarine B (2) and brevicalcarine C (3) were new C-19-diterpenoid alkaloid with an acetoxy group at C-18. In addition, the anti-neuroinflammatory activity of these compounds against BV-2 cells was investigated, which showed that none of them had significant anti-neuroinflammatory activity.