Value of the Data •Madagascar periwinkle (Catharanthus roseus) and drumstick tree leaves (Moringa oleifera) have been used in traditional medicine and their influence in various biomedical areas include antioxidant effects, hypolipidemic, anti-inflammatory, immunomodulatory, anti-hyperglycemic (anti-diabetic), anti-carcinogenic, anti-ulcer, anti-bacterial and also to treat few diseases such as Ocular, Alzheimer's and Parkinson disease. •Although quite a body of literature is available on Madagascar periwinkle and drumstick tree, the tentatively identified natural compounds with therapeutic potential may be exploited by the researchers for further investigations. •These data add to a growing body of evidence on the biological activities of extracts from these plants. Compounds reported in our GC-MS profiling may be applied in treating Tuberculosis, Non-small-cell lung cancer and to design rationalized drugs.