Nd5Fe92B3alloy was induction-melted. The α-Fe compounded low content of Nd2Fe14B nanocomposites were prepared using a melt-spinning method, subsequent annealing treatment, and ball milling. The complex permittivity, permeability of composites was measured in the 0.5-18 GHz frequency range. The permeability spectra exhibits relaxation type characteristic. The α-Fe/Nd2Fe14B composites shows an excellent microwave absorption property (reflection loss: RL<-20dB) in 9-17GHz with thin matching thickness 1.6-2.5 mm, due to the cooperate effect of magnetic loss and dielectric loss. α-Fe/Nd2Fe14B nanocomposites are thought to be a good microwave absorbers in GHz microwave range.