Carotenoid cleavage produces a variety of molecules, some of which are relatively small and nonpolar, and therefore of volatile nature at room temperature. These so-called volatile apocarotenoids are responsible, together with other volatiles, for the aroma of many plant products, and are key determinants of food flavor, often making an important contribution to the human perception of this attribute. Within the wide range of volatile molecules associated with food products, those derived from carotenoids tend to be perceived by our olfactory system as pleasant, many of them providing floral or fruity notes. Here we describe two methods for the determination of volatile apocarotenoids in two different plant organs: fruit and leaves. These methods include the extraction by means of headspace solid-phase microextraction (HS-SPME), followed by separation, detection, and quantification by means of gas chromatography coupled with mass spectrometry (GC-MS). The first method is exemplified for the case of a metabolically enriched tomato fruit, one of the most extensively consumed food products in our diet; the second method is exemplified for the analysis of spinach leaves, another widely consumed leafy vegetable.