The growing prominence of nutrition-related health problems demands strategies that explore nontraditional natural ingredients to expand healthy food alternatives. Specialty sorghums were decorticated using a tangential abrasive dehulling device (TADD) to remove successive bran layers, which were collected at 1 min intervals and analyzed for phenols, tannins, 3-deoxyanthocyanins, dietary fiber, and antioxidant activity. The first two bran fractions had the highest levels of phenols and antioxidant activity (3-6 times as compared to whole grain). Brown (tannin-containing) and black sorghums had at least 10 times higher antioxidant activity than white sorghum or red wheat brans. Black sorghums had the highest 3-deoxyanthocyanin content (up to 19 mg/g bran). Dietary fiber in sorghum brans ranged between 36 and 45%, as compared to 48% for wheat bran. Specialty sorghum brans are rich in valuable dietary components and present promising opportunities for improving health attributes of food.