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BaSr2Ca crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two BaSr2Ca ribbons oriented in the (0, 1, 0) direction. Ba is bonded in a linear geometry to two equivalent Sr atoms. Both Ba–Sr bond lengths are 3.77 Å. Sr is bonded in a linear geometry to one Ba and one Ca atom. The Sr–Ca bond length is 4.03 Å. Ca is bonded in a linear geometry to two equivalent Sr atoms.
BaSr2Ca 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 Sr atoms. All Ba–Sr bond lengths are 4.08 Å. Sr is bonded in a body-centered cubic geometry to four equivalent Ba and four equivalent Ca atoms. All Sr–Ca bond lengths are 4.08 Å. Ca is bonded in a body-centered cubic geometry to eight equivalent Sr atoms.