Three new alkaloids, 3-O-acetylveralkamine (1), veralkamine 3-(beta-D-glucopyranoside) (2), and 6,7-epoxyverdine (3), together with five known alkaloids, veramitaline, veralkamine (4), angeloylzygadenine, veratroylzygadenine, and veramiline 3-(beta-D-glucopyranoside), were isolated from the whole plants of Veratrum taliense. Their structures were elucidated on the basis of spectroscopic analysis, and the NMR data of veralkamine (4) are given for the first time. In addition, the cytotoxic activities of all isolated compounds, except for veramitaline, were tested.