The influence of Ga addition on the crystallization behavior and the magnetic properties of nanocomposite Nd2Fe14B-based/α-Fe magnets was investigated. It was found that the addition of 0.2% did not change the crystallization temperature of amorphous alloy, but the magnetic properties were improved significantly because of the strong exchange coupling interaction between the hard and soft magnetic phases. The optimum magnetic properties with iHc=600.3 kA·m-1, Br＝0.75 T, and (BH)max=88.03 kJ·m-3 were obtained in bonded Nd9.5(FeCoZr)83.8Ga0.2B6.5 magnet with 15 m·s-1 wheel speed and 670 ℃ annealing treatment. The apparent improvement of magnetic properties originates from the grain refinement calculated using the Scherrer formula from corresponding XRD patterns and the excellent rectangularity of the demagnetization curve.