Different pigmented corn and sorghum types were evaluated to characterize their biophysical, nutraceutical, and technofunctional properties for the first time. Commercially pigmented (blue, purple, red, black, and yellow) popcorn (Zea mays var. everta) and sorghum (Sorghum bicolor L.) of yellow and red colors were analyzed. Biophysical and proximal analyses were performed using official methods. The nutraceutical profile included the total phenolic and anthocyanin content. In addition, rheological, structural, and morphological studies were conducted. The results demonstrated significant differences between the popcorn samples and grain types, especially in terms of their biophysical and proximate features. The nutraceutical profile revealed that these specialty grains contained higher concentrations of antioxidant compounds (up to 3-fold when compared with the other grains). The rheological analysis demonstrated that sorghum grains developed higher peak viscosities than popcorn. According to the structural assessments, the type A pattern displayed peaks at the interplanar spaces corresponding to the crystalline and amorphous regions in all the samples. The data obtained in this study provides a base to further investigate the products obtained using these biomaterials.