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TbTl is Tetraauricupride structured and crystallizes in the cubic Pm-3m space group. The structure is three-dimensional. Tb is bonded in a body-centered cubic geometry to eight equivalent Tl atoms. All Tb–Tl bond lengths are 3.30 Å. Tl is bonded in a body-centered cubic geometry to eight equivalent Tb atoms.
TbTl(PSe3)2 crystallizes in the monoclinic P2_1 space group. The structure is three-dimensional. Tb3+ is bonded in a 8-coordinate geometry to eight Se2- atoms. There are a spread of Tb–Se bond distances ranging from 2.99–3.13 Å. Tl1+ is bonded in a 9-coordinate geometry to nine Se2- atoms. There are a spread of Tl–Se bond distances ranging from 3.29–3.94 Å. There are two inequivalent P4+ sites. In the first P4+ site, P4+ is bonded in a trigonal non-coplanar geometry to three Se2- atoms. There are a spread of P–Se bond distances ranging from 2.16–2.25 Å. In the second P4+ site, P4+ is bonded in a trigonal non-coplanar geometry to three Se2- atoms. There are a spread of P–Se bond distances ranging from 2.19–2.25 Å. There are six inequivalent Se2- sites. In the first Se2- site, Se2- is bonded in a 4-coordinate geometry to one Tb3+, two equivalent Tl1+, and one P4+ atom. In the second Se2- site, Se2- is bonded in a 1-coordinate geometry to one Tb3+, two equivalent Tl1+, and one P4+ atom. In the third Se2- site, Se2- is bonded in a 3-coordinate geometry to two equivalent Tb3+, one Tl1+, and one P4+ atom. In the fourth Se2- site, Se2- is bonded in a 1-coordinate geometry to three equivalent Tl1+ and one P4+ atom. In the fifth Se2- site, Se2- is bonded in a 3-coordinate geometry to two equivalent Tb3+ and one P4+ atom. In the sixth Se2- site, Se2- is bonded in a distorted trigonal non-coplanar geometry to two equivalent Tb3+, one Tl1+, and one P4+ atom.