From the leaves of Adhatoda vasica, the pyrrolo[2,1 b]quinazoline alkaloids l-vasicine [1], l-vasicinone [2], l-vasicol [3], anisotine [7], 3-hydroxyanisotine [8], and a new alkaloid, vasnetine [9] have been isolated and their structures established by ¹H- and ¹³C-nmr spectral studies. The chemical shift assignments for these alkaloids were confirmed by ¹H homonuclear COSY, DEFT, HETCOR, selective INEPT and HMBC nmr experiments.