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The chemical composition of the essential oils obtained from the leaves and roots of Cochlospermum angolense (Welw) growing wild in Angola was analyzed for the first time by capillary gas chromatography (GC) and gas chromatography/mass spectrometry (GC-MS). The investigation led to the identification of 67 and 130 compounds from the leaves and roots, respectively. Both oils were strongly characterized by the presence of sesquiterpenoids (68.8% in the leaves and 53.2% in the roots), while monoterpenoids were present in minor percentages (9.8% in the leaves and 26.2% in the root). The main constituents of the leaves were germacrene D (9.4%), alpha-cadinol (7.4%) and 10-epi-cubenol (6.2%), while the most abundant compounds in the root essential oil were the sesquiterpenes beta-caryophyllene (19.7%) and isoborneol (6.6%). The analysis by HS-SPME of the roots, leaves, fruits and seeds were also reported for the first time. Different volatile profiles were detected.