In general, there is a trade-off between magnetization and coercivity in nanocomposite magnets. Here, we demonstrate a simultaneous enhancement of both the magnetization and coercivity in bulk α-Fe/Nd₂Fe₁₄B nanocomposite magnets prepared via a severe plastic deformation (SPD) compared with thermally annealed magnets. The enhanced magnetization results from a high fraction (>30%) of α-Fe phase induced by SPD, while the increase in coercivity from 4.6 to 7.2 kOe is attributed to an enhancement in domain wall pinning strength. This study shows an increase in energy product is possible in the nanocomposite magnets for a large inclusion of soft-magnetic phase.