The Mo-content dependence of structure and magnetic properties of ( , 2, 3, 4, 5) nanocrystalline materials has been studied. The samples consist of hard-magnetic and soft-magnetic Co phases. The substitution of Mo for Co restrains the formation of Co, raises the content of , and increases the mean grain size of . Therefore, the coercive force of the sample increases with x. A coercive force of 7.9 kOe, which is a highest value reported among Zr-Co alloys, was achieved for . The anisotropy field of remains almost unchanged with increasing Mo content.