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TlI crystallizes in the orthorhombic Cmcm space group. The structure is three-dimensional. Tl1+ is bonded in a 5-coordinate geometry to seven equivalent I1- atoms. There are a spread of Tl–I bond distances ranging from 3.39–4.06 Å. I1- is bonded in a 5-coordinate geometry to seven equivalent Tl1+ atoms.
TlI 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 I1- atoms. All Tl–I bond lengths are 3.71 Å. I1- is bonded in a body-centered cubic geometry to eight equivalent Tl1+ atoms.
TlI3 crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. Tl3+ is bonded in a 5-coordinate geometry to five I1- atoms. There are a spread of Tl–I bond distances ranging from 3.63–3.76 Å. There are three inequivalent I1- sites. In the first I1- site, I1- is bonded in a 2-coordinate geometry to two I1- atoms. There are one shorter (2.88 Å) and one longer (3.03 Å) I–I bond lengths. In the second I1- site, I1- is bonded in a 1-coordinate geometry to four equivalent Tl3+ and one I1- atom. In the third I1- site, I1- is bonded in a 2-coordinate geometry to one Tl3+ and one I1- atom.
TlI is Halite, Rock Salt structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Tl1+ is bonded to six equivalent I1- atoms to form a mixture of edge and corner-sharing TlI6 octahedra. The corner-sharing octahedral tilt angles are 0°. All Tl–I bond lengths are 3.57 Å. I1- is bonded to six equivalent Tl1+ atoms to form a mixture of edge and corner-sharing ITl6 octahedra. The corner-sharing octahedral tilt angles are 0°.