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CsRb2Bi crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two CsRb2Bi ribbons oriented in the (0, 1, 0) direction. Cs is bonded in a linear geometry to two equivalent Rb atoms. Both Cs–Rb bond lengths are 4.76 Å. Rb is bonded in a distorted linear geometry to one Cs and one Bi atom. The Rb–Bi bond length is 3.58 Å. Bi is bonded in a linear geometry to two equivalent Rb atoms.
CsRb2Bi is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Cs is bonded in a 8-coordinate geometry to eight equivalent Rb and six equivalent Bi atoms. All Cs–Rb bond lengths are 4.00 Å. All Cs–Bi bond lengths are 4.61 Å. Rb is bonded to four equivalent Cs and four equivalent Bi atoms to form a mixture of distorted face, edge, and corner-sharing RbCs4Bi4 tetrahedra. All Rb–Bi bond lengths are 4.00 Å. Bi is bonded in a body-centered cubic geometry to six equivalent Cs and eight equivalent Rb atoms.