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CaOs3 is Uranium Silicide-like structured and crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Ca2+ is bonded to twelve equivalent Os+0.67- atoms to form a mixture of face and corner-sharing CaOs12 cuboctahedra. There are six shorter (2.89 Å) and six longer (2.90 Å) Ca–Os bond lengths. Os+0.67- is bonded in a distorted see-saw-like geometry to four equivalent Ca2+ atoms.
Ca3Os is alpha bismuth trifluoride structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. there are two inequivalent Ca sites. In the first Ca site, Ca is bonded to four equivalent Ca and four equivalent Os atoms to form a mixture of distorted corner, edge, and face-sharing CaCa4Os4 tetrahedra. All Ca–Ca bond lengths are 3.19 Å. All Ca–Os bond lengths are 3.19 Å. In the second Ca site, Ca is bonded in a 8-coordinate geometry to eight equivalent Ca and six equivalent Os atoms. All Ca–Os bond lengths are 3.69 Å. Os is bonded in a distorted body-centered cubic geometry to fourteen Ca atoms.