In this paper, binary Nd-Co alloys with compositional range from Nd72.5Co27.5 to Nd50Co50 were successfully vitrified into glassy state by a melt-spinning method. The glass formability of the metallic glasses (MGs) was studied and the best glass former in the binary Nd-Co alloys was obtained. Magnetic properties of the MGs were measured. The compositional dependence of Curie temperature of the MGs was observed. The mechanism for the spin-glass-like behaviors and high coercivity at low temperature, and their influence on the magnetic entropy change of the MGs, were investigated.