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Madagascar, the world's fourth biggest island has an unique biodiversity. The interest on the phytochemical investigation of Malagasy plants and marine natural products started from the isolation of the potent anti-cancerous bisindole alkaloids: vinblastine and vincristine. In this paper, works published in the last two decades (1991-2009) on 270 new natural products isolated from Madagascar higher plants, liverworts and marine organisms are reviewed. Several results on the bioassays of the isolated new natural products have been reported.