Two new monoterpenoid indole alkaloids, melohenryines A and B (1 and 2), along with six known indole alkaloids, were isolated from the twigs and leaves of Melodinus henryi. Structures of the new alkaloids were established by extensive spectroscopic techniques including NMR spectroscopy and mass spectrometry. Melohenryine A (1) represents the first example of monoterpenoid indole alkaloids characterized an ester carbonyl group at C-19 position. All of the new compounds were evaluated for in vitro cytotoxicity against several human cancer cell lines.