α-Fe coated Nd-Fe-B nano-composite magnetic powders were prepared by chemical vapor deposition (CVD), which were then spark plasma sintered to obtain Nd-Fe-B/α-Fe nano-composite magnets. SEM, XRD and XPS researches show that CVD method can realize uniform coating of Nd-Fe-B powders with α-Fe, improve effectively the distribution of hard and soft magnetic properties, and increase the integrated magnetic properties of the magnets. The obtained coating was dense and uniform, and the particle size of α-Fe was about 50-100 nm, when the temperature of CVD was 120 oC and the time was 30 min. Under optimum processing conditions, the SPSed NdFeB magnet can be nearly fully dense and reach the best magnetic properties with Br of 0.81 T, Hcj of 1286 kA/ m and (BH)m of 108.6 kJ/m3