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A method was developed for the isolation of geranyl acetate from the crude essential oil (EO) of Melaleuca armillaris (Sol. ex Gaertn.) Sm. leaves, and the purity of the isolated compound was analyzed by GC/MS spectral and NMR analysis and was found to have high purity (98.9%). In addition, the EO isolated presented 0.907 g/cm3, 1.474 and [ α ] D 20 = − 17.6 of density, refraction index and optical rotation, respectively. The chemical composition of the EO obtained for steam distillation from M. armillaris was analyzed by gas chromatographic and spectroscopic techniques (GC/MS and GC/FID). Thirty-eight compounds were identified, representing 99.92% of the total EO analyzed on a DB-5 ms (5% phenylmethylpolysiloxane) capillary column. This analysis showed that the EO consisted mainly of oxygenated monoterpenes (77.01%), followed by monoterpene hydrocarbons (21.31%) and sesquiterpene hydrocarbons (1.31%). Furthermore, the essential oil of M. armillaris was rich in 1,8-cineol (67 ± 2%), followed by limonene (10 ± 1%), α-Terpineol (9 ± 1%) and α-Pinene (5 ± 1%). Finally, the results suggest that the geranyl acetate isolated with high purity from crude essential oil is recommended to be explored as a component in medicinal or industrial use. [ABSTRACT FROM AUTHOR]