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ThOs2 is Cubic Laves structured and crystallizes in the cubic Fd-3m space group. The structure is three-dimensional. Th4+ is bonded in a 12-coordinate geometry to twelve equivalent Os2- atoms. All Th–Os bond lengths are 3.21 Å. Os2- is bonded to six equivalent Th4+ and six equivalent Os2- atoms to form a mixture of corner, edge, and face-sharing OsTh6Os6 cuboctahedra. All Os–Os bond lengths are 2.73 Å.
Th7Os3 crystallizes in the hexagonal P6_3mc space group. The structure is three-dimensional. there are three inequivalent Th sites. In the first Th site, Th is bonded in a distorted water-like geometry to two equivalent Os atoms. Both Th–Os bond lengths are 2.87 Å. In the second Th site, Th is bonded in a 3-coordinate geometry to three equivalent Os atoms. There are two shorter (2.89 Å) and one longer (3.05 Å) Th–Os bond lengths. In the third Th site, Th is bonded in a 3-coordinate geometry to three equivalent Os atoms. All Th–Os bond lengths are 2.95 Å. Os is bonded in a 6-coordinate geometry to six Th atoms.