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VOs is Tetraauricupride structured and crystallizes in the cubic Pm-3m space group. The structure is three-dimensional. V2+ is bonded in a body-centered cubic geometry to eight equivalent Os2- atoms. All V–Os bond lengths are 2.62 Å. Os2- is bonded in a body-centered cubic geometry to eight equivalent V2+ atoms.
VOs crystallizes in the hexagonal P-6m2 space group. The structure is three-dimensional. V2+ is bonded in a 6-coordinate geometry to six equivalent Os2- atoms. All V–Os bond lengths are 2.66 Å. Os2- is bonded to six equivalent V2+ atoms to form a mixture of distorted edge, face, and corner-sharing OsV6 cuboctahedra.
V4Os crystallizes in the orthorhombic Fmmm space group. The structure is three-dimensional. there are two inequivalent V sites. In the first V site, V is bonded in a 2-coordinate geometry to two equivalent V and two equivalent Os atoms. Both V–V bond lengths are 2.54 Å. Both V–Os bond lengths are 2.58 Å. In the second V site, V is bonded in a distorted body-centered cubic geometry to eight V atoms. There are two shorter (2.54 Å) and four longer (2.67 Å) V–V bond lengths. Os is bonded in a 4-coordinate geometry to four equivalent V atoms.