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TbSi2 is hexagonal omega structure structured and crystallizes in the hexagonal P6/mmm space group. The structure is three-dimensional. Tb is bonded to twelve equivalent Si atoms to form a mixture of edge and face-sharing TbSi12 cuboctahedra. All Tb–Si bond lengths are 3.09 Å. Si is bonded in a 9-coordinate geometry to six equivalent Tb and three equivalent Si atoms. All Si–Si bond lengths are 2.37 Å.
TbSi2 is hexagonal omega structure-like structured and crystallizes in the tetragonal I4_1/amd space group. The structure is three-dimensional. Tb is bonded to twelve equivalent Si atoms to form a mixture of edge and face-sharing TbSi12 cuboctahedra. There are eight shorter (3.08 Å) and four longer (3.14 Å) Tb–Si bond lengths. Si is bonded in a 9-coordinate geometry to six equivalent Tb and three equivalent Si atoms. There are two shorter (2.35 Å) and one longer (2.40 Å) Si–Si bond lengths.