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HoAu4 crystallizes in the tetragonal I4/m space group. The structure is three-dimensional. Ho is bonded to twelve equivalent Au atoms to form a mixture of edge and face-sharing HoAu12 cuboctahedra. There are eight shorter (3.02 Å) and four longer (3.04 Å) Ho–Au bond lengths. Au is bonded to three equivalent Ho atoms to form a mixture of distorted edge and corner-sharing AuHo3 cuboctahedra.
Ho2Au is Cotunnite structured and crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. there are two inequivalent Ho sites. In the first Ho site, Ho is bonded in a 3-coordinate geometry to five equivalent Au atoms. There are a spread of Ho–Au bond distances ranging from 2.94–3.63 Å. In the second Ho site, Ho is bonded to four equivalent Au atoms to form a mixture of edge and corner-sharing HoAu4 tetrahedra. There are a spread of Ho–Au bond distances ranging from 2.89–3.05 Å. Au is bonded in a 9-coordinate geometry to nine Ho atoms.