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GdTl is Tetraauricupride structured and crystallizes in the cubic Pm-3m space group. The structure is three-dimensional. Gd is bonded in a body-centered cubic geometry to eight equivalent Tl atoms. All Gd–Tl bond lengths are 3.34 Å. Tl is bonded in a body-centered cubic geometry to eight equivalent Gd atoms.
GdTl3 is Uranium Silicide structured and crystallizes in the cubic Pm-3m space group. The structure is three-dimensional. Gd is bonded to twelve equivalent Tl atoms to form GdTl12 cuboctahedra that share corners with twelve equivalent GdTl12 cuboctahedra, edges with twenty-four equivalent TlGd4Tl8 cuboctahedra, faces with six equivalent GdTl12 cuboctahedra, and faces with twelve equivalent TlGd4Tl8 cuboctahedra. All Gd–Tl bond lengths are 3.40 Å. Tl is bonded to four equivalent Gd and eight equivalent Tl atoms to form distorted TlGd4Tl8 cuboctahedra that share corners with twelve equivalent TlGd4Tl8 cuboctahedra, edges with eight equivalent GdTl12 cuboctahedra, edges with sixteen equivalent TlGd4Tl8 cuboctahedra, faces with four equivalent GdTl12 cuboctahedra, and faces with fourteen equivalent TlGd4Tl8 cuboctahedra. All Tl–Tl bond lengths are 3.40 Å.
Gd2Tl crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. there are two inequivalent Gd sites. In the first Gd site, Gd is bonded to six equivalent Gd and five equivalent Tl atoms to form a mixture of distorted face and corner-sharing GdGd6Tl5 trigonal bipyramids. All Gd–Gd bond lengths are 3.59 Å. There are three shorter (3.16 Å) and two longer (3.41 Å) Gd–Tl bond lengths. In the second Gd site, Gd is bonded in a 6-coordinate geometry to eight Gd and six equivalent Tl atoms. Both Gd–Gd bond lengths are 3.41 Å. All Gd–Tl bond lengths are 3.59 Å. Tl is bonded in a 11-coordinate geometry to eleven Gd atoms.