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Cs2Se is Fluorite structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Cs1+ is bonded to four equivalent Se2- atoms to form a mixture of corner and edge-sharing CsSe4 tetrahedra. All Cs–Se bond lengths are 3.68 Å. Se2- is bonded in a body-centered cubic geometry to eight equivalent Cs1+ atoms.
Cs2Se is Cuprite structured and crystallizes in the cubic Pn-3m space group. The structure is three-dimensional. Cs1+ is bonded in a linear geometry to two equivalent Se2- atoms. Both Cs–Se bond lengths are 3.41 Å. Se2- is bonded to four equivalent Cs1+ atoms to form corner-sharing SeCs4 tetrahedra.
Cs2Se crystallizes in the monoclinic P2_1 space group. The structure is three-dimensional. there are two inequivalent Cs1+ sites. In the first Cs1+ site, Cs1+ is bonded in a distorted rectangular see-saw-like geometry to four equivalent Se2- atoms. There are a spread of Cs–Se bond distances ranging from 3.69–3.88 Å. In the second Cs1+ site, Cs1+ is bonded in a 4-coordinate geometry to four equivalent Se2- atoms. There are a spread of Cs–Se bond distances ranging from 3.54–3.92 Å. Se2- is bonded in a 8-coordinate geometry to eight Cs1+ atoms.