Two new alkaloids, taberdines L (1) and M (2), together with six known alkaloids, were isolated from the twigs and leaves of Tabernaemontana divaricata. Taberdine L (1) represents the first optically active natural member of the allo iboga class of alkaloids with the ethyl side chain in a bridgehead position. Their structures including absolute configuration were elucidated by a combination of MS, NMR, and ECD calculation. The in vitro cytotoxic activities of 1 and 2 against five human cancer cell lines were also evaluated.