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HoSi2 is hexagonal omega structure structured and crystallizes in the hexagonal P6/mmm space group. The structure is three-dimensional. Ho is bonded to twelve equivalent Si atoms to form a mixture of edge and face-sharing HoSi12 cuboctahedra. All Ho–Si bond lengths are 3.07 Å. Si is bonded in a 9-coordinate geometry to six equivalent Ho and three equivalent Si atoms. All Si–Si bond lengths are 2.36 Å.
HoSi2 is hexagonal omega structure-like structured and crystallizes in the orthorhombic Imma space group. The structure is three-dimensional. Ho is bonded to twelve Si atoms to form a mixture of edge and face-sharing HoSi12 cuboctahedra. There are a spread of Ho–Si bond distances ranging from 3.04–3.17 Å. There are two inequivalent Si sites. In the first Si site, Si is bonded in a 9-coordinate geometry to six equivalent Ho and three Si atoms. There are two shorter (2.34 Å) and one longer (2.41 Å) Si–Si bond lengths. In the second Si site, Si is bonded in a 9-coordinate geometry to six equivalent Ho and three Si atoms. Both Si–Si bond lengths are 2.34 Å.