Structural and functional properties of starches from ensete pseudostems and water caltrop fruits were characterized and compared with other root and tuber (yam bean, taro, and cassava) and legume (chickpea and mungbean) starches. Taro and ensete starch granules were the smallest and largest, at respectively 2 μm and 42 μm average diameter. Amylose content varied from 7.91% in taro starch to 35.59% in chickpea starch with 19.20 and 20.85% in water caltrop and ensete starches. RVA analysis indicated that only water caltrop, mungbean, and chickpea starches had positive setback from peak, indicating strong gel formation. The dynamic rheological analysis also revealed high storage modulus (G′) values upon cooling for these three starches. Ensete starch granules had the lowest susceptibility to α-amylase hydrolysis. Principal component analysis (PCA) confirmed substantial differences between the functional properties of these starches. These results demonstrate the potential of atypical starches to find value-added uses as food ingredients, either in pure form or as blends of various starches.