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Interest in gluten-free grains is increasing, together with major incidences of celiac disease in the last years. Since to date, knowledge of the nutritional and bioactive compounds profile of alternative gluten-free grains is limited, we evaluated the content of water-soluble (thiamine and riboflavin) and liposoluble vitamins, such as carotenoids and tocols (tocopherols and tocotrienols), of gluten-free minor cereals and also of pseudocereals. The analysed samples showed a high content of bioactive compounds; in particular, amaranth, cañihua and quinoa are good sources of vitamin E, while millet, sorghum and teff (Eragrostis tef, or William’s Lovegrass) are good sources of thiamine. Moreover, millet provides a fair amount of carotenoids, and in particular of lutein. These data can provide more information on bioactive compounds in gluten-free grains. The use of these grains can improve the nutritional quality of gluten-free cereal-based products, and could avoid the monotony of the celiac diet.