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SiSe2 is Cyanogen Chloride-derived structured and crystallizes in the orthorhombic Ibam space group. The structure is zero-dimensional and consists of four $l^{1}-selanyl(selanylidene)silicon molecules. Si4+ is bonded in a linear geometry to two equivalent Se2- atoms. Both Si–Se bond lengths are 2.09 Å. Se2- is bonded in a single-bond geometry to one Si4+ atom.
Si3Se is alpha bismuth trifluoride structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. there are two inequivalent Si+1.33- sites. In the first Si+1.33- site, Si+1.33- is bonded in a distorted body-centered cubic geometry to four equivalent Si+1.33- and four equivalent Se4+ atoms. All Si–Si bond lengths are 2.78 Å. All Si–Se bond lengths are 2.78 Å. In the second Si+1.33- site, Si+1.33- is bonded in a body-centered cubic geometry to eight equivalent Si+1.33- atoms. Se4+ is bonded in a body-centered cubic geometry to eight equivalent Si+1.33- atoms.