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TlBr is Tetraauricupride structured and crystallizes in the cubic Pm-3m space group. The structure is three-dimensional. Tl1+ is bonded in a body-centered cubic geometry to eight equivalent Br1- atoms. All Tl–Br bond lengths are 3.51 Å. Br1- is bonded in a body-centered cubic geometry to eight equivalent Tl1+ atoms.
TlTlBr4 is Iron carbide-like structured and crystallizes in the orthorhombic Pnna space group. The structure is zero-dimensional and consists of four thallium molecules and four TlBr4 clusters. In each TlBr4 cluster, Tl is bonded in a tetrahedral geometry to four Br atoms. There are two shorter (2.63 Å) and two longer (2.64 Å) Tl–Br bond lengths. There are two inequivalent Br sites. In the first Br site, Br is bonded in a single-bond geometry to one Tl atom. In the second Br site, Br is bonded in a single-bond geometry to one Tl atom.
TlBr crystallizes in the orthorhombic Cmcm space group. The structure is three-dimensional. Tl1+ is bonded in a 5-coordinate geometry to seven equivalent Br1- atoms. There are a spread of Tl–Br bond distances ranging from 3.21–3.84 Å. Br1- is bonded in a 5-coordinate geometry to seven equivalent Tl1+ atoms.
(Tl)3Br crystallizes in the hexagonal P6_3/mmc space group. The structure is zero-dimensional and consists of two hydrobromic acid molecules and six thallium molecules.