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PuOs2 is Cubic Laves structured and crystallizes in the cubic Fd-3m space group. The structure is three-dimensional. Pu4+ is bonded in a 12-coordinate geometry to twelve equivalent Os2- atoms. All Pu–Os bond lengths are 3.09 Å. Os2- is bonded to six equivalent Pu4+ and six equivalent Os2- atoms to form a mixture of edge, face, and corner-sharing OsPu6Os6 cuboctahedra. All Os–Os bond lengths are 2.64 Å.
Pu5Os3 crystallizes in the orthorhombic Fmmm space group. The structure is three-dimensional. there are three inequivalent Pu sites. In the first Pu site, Pu is bonded to four Os atoms to form distorted edge-sharing PuOs4 tetrahedra. There are two shorter (2.71 Å) and two longer (2.72 Å) Pu–Os bond lengths. In the second Pu site, Pu is bonded in a 6-coordinate geometry to six Os atoms. There are a spread of Pu–Os bond distances ranging from 2.94–3.19 Å. In the third Pu site, Pu is bonded in a 6-coordinate geometry to six Os atoms. There are a spread of Pu–Os bond distances ranging from 2.93–3.19 Å. There are three inequivalent Os sites. In the first Os site, Os is bonded in a 10-coordinate geometry to eight Pu and two equivalent Os atoms. Both Os–Os bond lengths are 2.77 Å. In the second Os site, Os is bonded in a 10-coordinate geometry to ten Pu atoms. In the third Os site, Os is bonded in a 10-coordinate geometry to ten Pu atoms.