We report the core/shell type as the interesting one of the various techniques to prepare exchange-coupled permanent magnet. In this study, the exchange-coupled Nd2Fe14B/α-Fe was prepared by high energy ball mill process and chemical reduction. Nd15Fe77B8 powder prepared by high energy ball mill process was coated with α-Fe nanoparticle by chemical reduction. α-Fe nanoparticle on the ball milled Nd15Fe77B8 was synthesized by chemical reduction with borohydride as a reducing agent in aqueous solution. After annealing, Nd2Fe14B/α-Fe forming core/shell shape has exchange-coupling effect and was identified by using XRD, FE-SEM, VSM, TMA and EDX.