Gas chromatography (GC) is recognized as a powerful tool not only for analysis of volatile but also for semi- and non-volatile components present in traditional Chinese medicines (TCMs). When coupled with mass spectrometry (MS), it could afford rather abundant structural information of the components in TCMs. In this study, the strategies for quantification, including reference compounds, sample preparation and analytical approaches, in quality control of TCMs by GC-MS were focused on. The major achievements of this study are summarized as follows: (1) A fast and reliable method based on supercritical fluid extraction (SFE) and molecular distillation (MD) was established for the preparation of standardized reference extract (SRE) of Curcuma longa. The SRE based quantitative evaluation of multiple analytes was successfully applied to easily and effectively control the quality of C. longa L. by GC-MS. (2) Glycome of Astragalus membranaceus (Fisch.) Bge. var. mongholicus (Bge.) Hsiao including free and polymeric carbohydrates were qualitatively and quantitatively analyzed based on optimized pressurized liquid extraction (PLE), microwave-assisted acidic hydrolysis (MAAH) and GC-MS coupled with different chromatographic approaches. Twelve saccharides, including sucrose, galacturonic acid, mannitol, fructose, rhamnose, ribose, arabinose, fucose, xylose, mannose, glucose and galactose were successfully quantified by GC-MS and HPLC-CAD (charged aerosol detectors). Different columns were compared for evaluation of oligosaccharides. The polysaccharides in water extract of A. membranaceus (Fisch.) Bge. var. mongholicus (Bge.) Hsiao were also characterized by high performance size exclusive chromatography (HPSEC) combined with multiple angle light scattering detection (MALSD) and refractive index detection (RID). The glycome of A. membranaceus (Fisch.) Bge. var. mongholicus (Bge.) Hsiao was successfully decoded by the established GC-MS method coupled with different chromatographic approaches (3) A one step derivatization method coupled with GC-MS was developed for simultaneous analysis of fatty acids and sterols and successfully applied for discriminating the multi-origin TCMs Ganoderma, G. sinense and G. lucidum listed in Chinese Pharmacopeia. In summary, a SRE was prepared and applied for quality control of volatile components in C. longa by GC-MS; the glycome of A. membranaceus (Fisch.) Bge. var. mongholicus (Bge.) Hsiao was decoded by optimized sample preparation methods and selected chromatographic approaches; and G. sinense and G. lucidum were successfully discriminated based on one step derivatization method coupled with GC-MS, all of which provided powerful tools for quality control of these plants.