The natural fragrance compounds produced by plants play key roles in the long-term fitness and survival of these plants as well as being of direct/indirect benefit to man. Almost all plant fragrances, either pleasant or unpleasant, comprise many different compounds, from different chemical classes and can indeed be highly complex in composition involving several hundred types of volatile molecule. Analyzing these mixtures and identifying their main (bio)active components is of importance in both fundamental and applied science. Gas Chromatography-Mass Spectrometry (GC-MS) plays a central role here. GC-MS has regularly been used for fragrance analysis and different extraction/adsorption and detection protocols have been designed specifically for plant materials. In this chapter, two methods are presented for two highly contrasting plant organs-a melon fruit and rice grains. Metabolomics analyses of these important food crops are already helping us understand better which components are most important in determining the flavour of these important food crops and how we might go about producing new "designer" crops which are even tastier than the existing ones.