Reinvestigation of the fruits of Alangium lamarckii has led to the isolation and structural determination of five new tetrahydroisoquinoline-monoterpene glucosides, methylisoalangiside [5], isoalangiside [6], 3-O-demethyl-2-O-methylisoalangiside [7], demethylneoalangiside [8], and neoalangiside [9], as well as a novel tetrahydro-β-carboline-monoterpene glucoside, 10-hydroxyvincoside lactam [10]. Demethylalangiside, sweroside, and phenethyl alcohol xylopyranosyl(1→6) glucopyranoside were also isolated for the first time from this plant. The structures of the new compounds were elucidated by spectroscopic and chemical methods. The biogenesis of these glucosides is also discussed.