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Tibetan hull-less barley grows at above 4,000 m altitude. One variety grown in the plain and three varieties grown in Tibet were collected from Tianjin and Lhasa. The barleys were polished into five fractions. Total soluble phenolic content (TSPC), total antioxidant capacity (TAC), and their correlation were investigated. Phenolic compounds were analyzed by HPLC, and TSPC content was evaluated by the Folin–Ciocalteu colorimetric method. TAC was measured using 2,2-diphenyl-1-picrylhydrazyl, 2,2'-azinobis-(3-ethylbenzthiazoline-6-sulfonate), and ferric reducing ability of plasma assays. Results showed that TSPC decreased from the outer to the inner fractions, with the outermost layer containing the highest (around 2,803–7,703 µg/g) and inner endosperm the lowest (around 870–1,348 µg/g). TSPC and TAC were highly and positively correlated (r= 0.9583–0.9710). Colored hull-less barley had higher antioxidant activity than uncolored. TSPC and TAC of Tibetan varieties in the outer layers were more than two-fold higher than that of Tianjin hull-less barley. Tibetan hull-less barley bran extracts are valuable sources of bioactive components with antioxidant activity.