NdNi2 is Cubic Laves structured and crystallizes in the cubic Fd-3m space group. The structure is three-dimensional. Nd is bonded in a 12-coordinate geometry to twelve equivalent Ni atoms. All Nd–Ni bond lengths are 3.03 Å. Ni is bonded to six equivalent Nd and six equivalent Ni atoms to form a mixture of corner, edge, and face-sharing NiNd6Ni6 cuboctahedra. All Ni–Ni bond lengths are 2.58 Å.