Four natural N-methylindolines have been isolated from the roots of Vinca sardoa (Stearn) Pignati. They are ent-N(1)-methyl-14,15-didehydroaspidospermidine (7),N(1)-methyl-14,15-didehydroaspidofractinine (10), N(1)-methylaspidofractinine (11) and N(1)-methyl-14,15-didehydrotuboxenine (13)