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Nb3Os crystallizes in the cubic Pm-3n space group. The structure is three-dimensional. Nb is bonded in a 6-coordinate geometry to two equivalent Nb and four equivalent Os atoms. Both Nb–Nb bond lengths are 2.59 Å. All Nb–Os bond lengths are 2.90 Å. Os is bonded to twelve equivalent Nb atoms to form a mixture of face and edge-sharing OsNb12 cuboctahedra.
Nb3Os is alpha bismuth trifluoride structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. there are two inequivalent Nb sites. In the first Nb site, Nb is bonded to four equivalent Nb and four equivalent Os atoms to form a mixture of distorted corner, edge, and face-sharing NbNb4Os4 tetrahedra. All Nb–Nb bond lengths are 2.81 Å. All Nb–Os bond lengths are 2.81 Å. In the second Nb site, Nb is bonded in a 8-coordinate geometry to eight equivalent Nb and six equivalent Os atoms. All Nb–Os bond lengths are 3.24 Å. Os is bonded in a distorted body-centered cubic geometry to fourteen Nb atoms.