Four indole alkaloids, alstonlarsines A-D (1-4), were isolated from Alstonia scholaris and structurally characterized. Compound 1 possesses a new carbon skeleton with a cage-shaped 9-azatricyclo[4.3.1.0(3,8)]decane motif, and compounds 2-4 feature a rare carbon skeleton that was found in nature for the first time. Plausible biosynthetic routes for 1-4 are proposed. Compound 1 showed DRAK2 inhibitory activity with an IC50 value of 11.65 +/- 0.63 mu M.