Carotenoids are among the most valuable food constituents in terms of food quality and human health effects. As natural pigments, they confer the pleasing yellow, orange, or red color of many fruits, vegetables, egg yolk, crustaceans, and some fish. The principal carotenoids found in foods are β-carotene, α-carotene, β-cryptoxanthin, lycopene, lutein, and zeaxanthin. These carotenoids are also the most commonly found in human plasma and have been the most studied in terms of health benefits. This chapter reviews the carotenoid compositions of three major staple foods consumed by millions of people in many countries, especially developing countries, along with their possible use in the fortification of flour and bakery products. For all three crops, nutrition education is needed to promote acceptability, considering the current preference for varieties devoid of color in many countries. For Orange-fleshed sweet potato (OFSP), varieties with considerable amounts of all-E-b-carotene are available; however, for cassava and maize, enhancing the provitamin A content is still being pursued, especially by biofortification, although adding β-carotene to cassava flour may be an alternative. The use of carotenoid-rich or biofortified flours in a variety of products has been shown to be technologically feasible; carotenoid retention during these processes needs to be demonstrated. © 2011 Elsevier Inc. 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