The volatile compounds from roots, stems, and leaves of Valeriana hardwickii and Valeriana officinalis were obtained by microdistillation and analyzed by gas chromatography-flame ionization detector (GC-FID) and gas chromatography-mass spectometry (GC-MS). In V. hardwickii, sixty-two, thirty-one, and thirty-one components were identified representing 90, 90, and 92% of total oil in the roots, stems, and leaves, respectively. The major compounds in the root oil were camphene (12.9%), bornyl acetate (17.6%), and maaliol (10.6%), while borneol (6.2%), trans-anethole (32.7%), and maaliol (6.3%) were the dominant components in the stem oil and camphene (12.6%), bornyl acetate (15.0%), and hexahydrofarnesyl acetone (9.2%) were the principal components in the leaf oil. In V. officinalis, bornyl acetate (7.8%), delta-elemene (9.3%), and valerenal (14.7%) were the dominant components in the roots among fifty-four compounds identified which accounted for 80% of the total oil. In contrast to V. hardwickii, the stems and roots of V. officinalis contained very small amounts of essential oil and consequently, only a few compounds were identified in the leaves and none could be detected in the stems.