Six undescribed alkaloids, neotuberostemonol C (1), dehydrostenines C-D (2-3), tuberostemonines Q-R (10-11), and (6R,8R,8aR)-8-hydroxy-6-methyl-hexahydroindolizin-5-one (32), along with twenty-six known analogues were isolated from the dried roots of Stemona tuberosa Lour. The structures and absolute stereochemistry of these compounds were delineated by extensive spectroscopy (1D NMR, 2D NMR, HRESIMS), quantum chemical calculations of the electronic circular dichroism spectra, and pyridine-induced solvent shifts. Tuberostemonines Q-R (10-11) represent tuberostemonine skeleton alkaloids possessing an alpha-methyl-gamma-butyrolactone moiety attached to C-3. In addition, all these isolated compounds were assayed for their inhibitory activity against LPS-induced NO production in RAW264.7 cells using Griess assay.