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ThBr4 crystallizes in the tetragonal I4_1/amd space group. The structure is three-dimensional. Th4+ is bonded in a 8-coordinate geometry to eight equivalent Br1- atoms. There are four shorter (2.89 Å) and four longer (3.13 Å) Th–Br bond lengths. Br1- is bonded in a distorted water-like geometry to two equivalent Th4+ atoms.
ThBr4 crystallizes in the tetragonal I4_1/a space group. The structure is three-dimensional. Th4+ is bonded in a 8-coordinate geometry to eight equivalent Br1- atoms. There are four shorter (2.95 Å) and four longer (3.05 Å) Th–Br bond lengths. Br1- is bonded in a water-like geometry to two equivalent Th4+ atoms.
Th3Br is Uranium Silicide-like structured and crystallizes in the tetragonal I4/mmm space group. The structure is three-dimensional. there are two inequivalent Th sites. In the first Th site, Th is bonded to four equivalent Br atoms to form a mixture of distorted edge and corner-sharing ThBr4 cuboctahedra. All Th–Br bond lengths are 3.51 Å. In the second Th site, Th is bonded in a square co-planar geometry to four equivalent Br atoms. All Th–Br bond lengths are 3.47 Å. Br is bonded to twelve Th atoms to form a mixture of edge, face, and corner-sharing BrTh12 cuboctahedra.