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HfSi crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. Hf4+ is bonded in a 7-coordinate geometry to seven equivalent Si4- atoms. There are a spread of Hf–Si bond distances ranging from 2.71–2.91 Å. Si4- is bonded in a 9-coordinate geometry to seven equivalent Hf4+ and two equivalent Si4- atoms. Both Si–Si bond lengths are 2.47 Å.
(HfSi)2CuSi crystallizes in the tetragonal P4/mmm space group. The structure is zero-dimensional and consists of one copper molecule, one silicon molecule, and two HfSi clusters. In each HfSi cluster, Hf is bonded in a single-bond geometry to one Si atom. The Hf–Si bond length is 2.31 Å. Si is bonded in a single-bond geometry to one Hf atom.