Seventeen cultivars of hard and soft spring wheat (Triticum aestivum L.), and 29 cultivars of two-row and six-row barley (Hordeum distichum and H. vulgare) were examined for bulk weight (BW), 1,000-kernel weight (KW) and plumpness, and analyzed for gross composition, amylose, gross energy (GE), β-glucan (barley only), and for sedimentation (wheat only). Digestion coefficients and digestible energy (DE) values of the cultivars were determined by mouse-feeding. The ranges in protein, starch, amylose, and GE varied from 5 to 15%, whereas ether extract, fiber, ash and β-glucan contents varied from 1 to 3%. Except for sedimentation in wheat, and plumpness in barley there were no major differences in physical or chemical characters between hard and soft wheats or between two- and six-row barley. In wheat, DE was significantly correlated with BW (−0.59, P < 0.05), KW (−0.53, P < 0.05), plumpness (−0.55, P < 0.05), fiber (+0.72, P < 0.01), ash (−0.52, P < 0.05), sedimentation (−0.57, P < 0.05) and GE (+0.97, P < 0.01). Digestion coefficient was significantly correlated with protein (−0.58, P < 0.05), ash (−0.56, P < 0.05), and sedimentation (−0.57, P < 0.05). In barley, DE was significantly correlated with protein (+0.41, P < 0.05) and GE (+0.82, P < 0.01), and digestion coefficient was significantly correlated with BW (+0.55, P < 0.01), plumpness (+0.45, P < 0.05), ether extract (+0.50, P < 0.01), and fiber (−0.52, P < 0.01). For use as selection criteria the most significant correlations were between DE and GE and sedimentation in wheat, and between DE and GE in barley.