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TmAu4 crystallizes in the tetragonal I4/m space group. The structure is three-dimensional. Tm is bonded to twelve equivalent Au atoms to form a mixture of edge and face-sharing TmAu12 cuboctahedra. There are eight shorter (3.00 Å) and four longer (3.03 Å) Tm–Au bond lengths. Au is bonded to three equivalent Tm atoms to form a mixture of distorted edge and corner-sharing AuTm3 cuboctahedra.
Tm2Au is Cotunnite structured and crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. there are two inequivalent Tm sites. In the first Tm site, Tm is bonded to four equivalent Au atoms to form a mixture of edge and corner-sharing TmAu4 tetrahedra. There are a spread of Tm–Au bond distances ranging from 2.87–3.00 Å. In the second Tm site, Tm is bonded in a 3-coordinate geometry to five equivalent Au atoms. There are a spread of Tm–Au bond distances ranging from 2.94–3.53 Å. Au is bonded in a 9-coordinate geometry to nine Tm atoms.