Three new monoterpenoid indole alkaloids, vinmajorines C-E (1-3), along with 18 known analogues (4-21), were isolated from the whole plants of Vinca major. The new structures were elucidated as (5α,15β,16R,17α,19β,20α,21β)-10,17-dimethoxy-21-methyl-18-oxa-5,16-cycloyohimban-19-ol (1), (5α,15β,16R,17α,20α,21β)-10-methoxy-21-methyl-18-oxa-5,16-cycloyohimban-17-ol (2), and (5α,15β,16R,17α,20α,21β)-10-methoxy-21-methyl-18-oxa-5,16-cycloyohimban-17-yl acetate (3), respectively, by extensive NMR and MS analysis and comparison with known compounds. Compounds 1-3 were evaluated for their cytotoxic activities against five human cancer cell lines, compounds 1 and 3 showing moderate cytotoxic activities. Copyright © 2016 Verlag Helvetica Chimica Acta AG, Zürich.