Samples of the sweet-tasting species Acanthospermum hispidum DC. (Compositae) (aerial parts), Boscia salicifolia Oliv. (Capparidaceae) (stem bark), Hovenia dulcis Thunb. (Rhamnaceae) (peduncles) and Inga spectabilis Willd. (Leguminosae) (arils) were acquired as part of a continuing search for high-intensity natural sweeteners of plant origin. Following their preliminary safety evaluation, the sweetness of these plants was traced to large amounts of sugars and polyols by taste-guided fractionation, which were identified and quantified using gas chromatography/mass spectrometry. The combined yields of sugars and polyols in the A. hispidum, B. salicifolia, H. dulcis, and I. spectabilis samples investigated were 6.9, 10.1, 18.4 and 12.1% w/w, respectively. These yields are much higher than the total saccharide and polyol content (2.4% w/w) of the sweet dried fruits of Thladiantha grosvenorii (Swingle) C. Jeffrey (Cucurbitaceae), a species which has previously been reported to contain more than 1% w/w of the intensely sweet triterpene, mogroside V. The dried leaves of Symplocos tinctoria (L.) L'Hérit. (Symplocaceae), which were not appreciably sweet, were found to contain only 2.0% w/w of sugars. The results of this investigation, therefore, suggest that unless the saccharide and/or polyol content of a plant part is well over 5% w/w, then it is unlikely to exhibit an overtly sweet taste, unless an intense sweetener is present.