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RbTl3 crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Rb is bonded in a 12-coordinate geometry to twelve equivalent Tl atoms. There are six shorter (3.93 Å) and six longer (4.19 Å) Rb–Tl bond lengths. Tl is bonded in a 2-coordinate geometry to four equivalent Rb and six equivalent Tl atoms. There are four shorter (3.33 Å) and two longer (3.39 Å) Tl–Tl bond lengths.
RbTl3 is alpha bismuth trifluoride structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Rb is bonded in a distorted body-centered cubic geometry to fourteen Tl atoms. There are eight shorter (3.57 Å) and six longer (4.12 Å) Rb–Tl bond lengths. There are two inequivalent Tl sites. In the first Tl site, Tl is bonded to four equivalent Rb and four equivalent Tl atoms to form a mixture of corner, edge, and face-sharing TlRb4Tl4 tetrahedra. All Tl–Tl bond lengths are 3.57 Å. In the second Tl site, Tl is bonded in a 6-coordinate geometry to six equivalent Rb and eight equivalent Tl atoms.