Dried flowers and leaves of four different Achillea species grown wild in several provinces of Iran, including one species collected from three different locations of Isfahan province were analyzed for the headspace volatile components, total phenolics (TP) and tartaric esters (TE). Capillary gas chromatography/mass spectrometry (GC/MS) combined with a purge and trap method was used for quantification of aroma components. Over 70 compounds were determined in the samples. Flower samples from all species contained 2-methyl butanal, alpha-pinene, alpha-thujene, camphene, hexanal, beta-pinene and 1,8-cineole; however, the major constituents of the aerial parts were determined as alpha-pinene, camphene, DL-limonene and 1,8-cineole. The largest number of aroma components were found in Achillea tenuifolia Lam. and Achillea millefolium L. In all species, except A. millefolium, the leaves contained more TP and TE than flowers. However, A. wilhelmsii from Semirom in Isfahan province showed the highest values for TP and TE.