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NdSi2 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 Si atoms. All Nd–Si bond lengths are 3.20 Å. Si is bonded to six equivalent Nd and six equivalent Si atoms to form a mixture of edge, face, and corner-sharing SiNd6Si6 cuboctahedra. All Si–Si bond lengths are 2.73 Å.
NdSi2 is hexagonal omega structure-like structured and crystallizes in the tetragonal I4_1/amd space group. The structure is three-dimensional. Nd is bonded to twelve Si atoms to form a mixture of face and edge-sharing NdSi12 cuboctahedra. There are four shorter (3.16 Å) and eight longer (3.19 Å) Nd–Si bond lengths. There are three inequivalent Si sites. In the first Si site, Si is bonded in a 9-coordinate geometry to six equivalent Nd and three Si atoms. There are one shorter (2.38 Å) and two longer (2.40 Å) Si–Si bond lengths. In the second Si site, Si is bonded in a 9-coordinate geometry to six equivalent Nd and three Si atoms. The Si–Si bond length is 2.38 Å. In the third Si site, Si is bonded in a 9-coordinate geometry to six equivalent Nd and three Si atoms.