The volatile compositions of hydrodistilled essential oils in the flower heads of Chrysanthemum indicum L. from eight populations in China were analyzed by GC/MS. A total of 169 compounds representing 88.79-99.53% of the oils were identified, and some remarkable differences were found in the constituent percentages of the eight populations. The predominant components of the essential oils were 1,8-cineole (0.62-7.34%), (+)-(1R,4R)-camphor (0.17-27.56%), caryophyllene oxide (0.54-5.8%), β-phellandrene (0.72-1.87%), (-)-(1S,2R,4S)-borneol acetate (0.33-8.46%), 2-methyl-6-(p-tolyl)hept-2-ene (0.3-8.6%), 4,6,6-trimethylbicyclo[3.1.1]hept-3-en-2-yl acetate (0.17-26.48%), and hexadecanoic acid (0.72-15.97%). The chemotaxonomic value of the essential-oil compositions was discussed according to the results of cluster analysis (CA) and principal-component analysis (PCA). The eight populations were divided into five groups as different chemotypes (Groups A-E), and the scores together with the loadings revealed clearly different chemical properties of each population. In conclusion, GC/MS in combination with chemometric techniques provided a flexible and reliable method for characterizing the essential oils of different populations of C. indicum L.