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BaSrTl2 crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two BaSrTl2 ribbons oriented in the (1, 0, 0) direction. Ba is bonded in a linear geometry to two equivalent Tl atoms. Both Ba–Tl bond lengths are 3.15 Å. Sr is bonded in a linear geometry to two equivalent Tl atoms. Both Sr–Tl bond lengths are 3.08 Å. Tl is bonded in a linear geometry to one Ba and one Sr atom.
BaSrTl2 is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Ba is bonded in a body-centered cubic geometry to eight equivalent Tl atoms. All Ba–Tl bond lengths are 3.66 Å. Sr is bonded in a body-centered cubic geometry to eight equivalent Tl atoms. All Sr–Tl bond lengths are 3.66 Å. Tl is bonded in a body-centered cubic geometry to four equivalent Ba and four equivalent Sr atoms.