The chemical investigation of the leaves of Hunteria zeylanica (Retz) Gardn. ex Thw. collected in Thailand resulted in the isolation of two new sarpagine-type indole alkaloids, Nb-methyl-3a-amino-seco-voacarpine (1) and hunteriatryptamine (3), along with twelve known bases. Hunteria zeylanica is a tropical plant of the Apocynaceae family, whose latex has been traditionally used for treating yaws sores, and its stem bark crude alkaloids exhibit antinociceptive, antipyretic, and anti-inflammatory effects. Further studies on the alkaloidal constituents of its leaves isolated two new minor alkaloids: seven alkaloids were obtained from the first collection in June 1992, including (1), and ten from the second in August 1993, including (3). Structural elucidation of (1) and (3) was performed using spectral techniques (UV, 1H/13C NMR, HR-EI/MS, HR-FAB/MS, COSY, PHSQC, HMBC, PROESY) and chemical analysis. Compound (1), a colorless solid with molecular formula C22H29N3O3, was identified as Nb-methyl-3a-amino-seco-voacarpine with S configuration at C-16, α-orientation of the amino group at C-3, and E configuration of the ethylidene side chain. Compound (3), an amorphous powder with molecular formula C32H39N4O3, was characterized as 16-hydroxymethylceridimine (named hunteriatryptamine) with α-orientation of the tryptamine unit at C-3 and E stereochemistry at C-19. The co-occurrence of these new alkaloids with coryzeylamine suggests a biogenetic pathway involving the quaternary alkaloid icepi-macusine A as a common precursor, though this precursor was not detected in the investigation.