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Ca2TlIn crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Ca2TlIn ribbons oriented in the (1, 0, 0) direction. Ca is bonded in a linear geometry to one Tl and one In atom. The Ca–Tl bond length is 3.19 Å. The Ca–In bond length is 3.17 Å. Tl is bonded in a linear geometry to two equivalent Ca atoms. In is bonded in a linear geometry to two equivalent Ca atoms.
Ca2TlIn is Heusler-like structured and crystallizes in the tetragonal P4/mmm space group. The structure is three-dimensional. Ca is bonded in a body-centered cubic geometry to four equivalent Tl and four equivalent In atoms. All Ca–Tl bond lengths are 3.36 Å. All Ca–In bond lengths are 3.35 Å. Tl is bonded in a body-centered cubic geometry to eight equivalent Ca atoms. In is bonded in a body-centered cubic geometry to eight equivalent Ca atoms.
Ca2TlIn is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Ca is bonded in a body-centered cubic geometry to four equivalent Tl and four equivalent In atoms. All Ca–Tl bond lengths are 3.37 Å. All Ca–In bond lengths are 3.37 Å. Tl is bonded in a body-centered cubic geometry to eight equivalent Ca atoms. In is bonded in a body-centered cubic geometry to eight equivalent Ca atoms.