The effect of substitution of Ni for Co in the borides Nd 3 (Co 13 Ni )B 2 ( = 0, 1, 2, 3, 4, 5) on the crystal structure and magnetic properties has been investigated. The lattice parameter decreases while increases with increasing in the range 0 5. The Curie temperature and saturation magnetic moment per formula unit in Nd 3 (Co 13 Ni )B 2 decrease monotonically as the Ni concentration increases. We have observed spin-reorientation transitions at temperatures that decrease monotonically with increasing Ni concentration. It is noteworthy that the substitution of Ni has a significant effect on the magnetocrystalline anisotropy of the Co sublattice, leading to the change of easy magnetization direction of Nd 3 (Co 13 Ni )B 2 compounds from basal plane to the axis at room temperature when 2. The magnetic phase diagram of the Nd 3 (Co 13 Ni )B 2 borides is given, and the behavior of magnetocrystalline anisotropy is analyzed by the single ion model.