Phytochemical investigation on the leaves of Neolamarckia cadamba led to the isolation of four new indole alkaloids, spirocadambine (1), dehydraisodihydrocadambine (2), nitrocadambines A and B (3 and 4). The structures and relative configurations were established by 1D and 2D NMR spectra. Spirocadambine (1) represents a new type of screw ring containing indole glucoalkaloids.