The coercivity enhancement of ball-milled Nd2Fe14B/α-Fe nanocomposite magnets was investigated. It was found that the coerciv- ity could be enhanced through mixing a small amount of Nd powder with as-milled Fe-rich Nd-Fe-B powders. The annealed samples were investigated by means of X-ray diffraction, scanning electron microscopy and magnetic measurement systems. Under annealing, some of Nd powders promoted the formation of hard magnetic phase Nd2Fe14B. On the other hand, a few of Nd would diffuse into the interface of Nd2FelaB/α-Fe nanocomposite to compensate for the loss of the interracial magnetic anisotropy. These two features are all beneficial to the coercivity.