Bran, a byproduct still mainly used for animal feed, is receiving increased attention as potential ingredient for a healthier diet. The aim of this study was to characterize and evaluate the nutritional and antioxidant properties of wheat and oat bran in order to promote their use as nutraceutical ingredients in flour and/or other products. The effects of grain (wheat vs. oat) and milling fraction (whole grain vs. bran) on the phenolic profile (free vs. bound phenolics), antioxidant and nutrient profiles, and glycemic index were evaluated. Differences in antioxidant capacity through different methodologies between grain and bran were observed, supporting a higher in vitro antioxidant capacity of the whole grain than that of the refined flours, which lack the bran fraction. The highest RACI (Relative Antioxidant Capacity Index) corresponded to wheat bran bound fraction, which showed the highest concentration of ferulic acid and correlation with antioxidant parameters tested. The in vitro glycemic index of the bran fractions was reduced, as compared with grain, with lower values found for wheat. The results support the important benefits of the polyphenols linked to fiber and the importance to develop methods to increase bioavailability of these compounds, which would promote WB use as nutraceutical ingredient.