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PuSb3 crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Pu3+ is bonded to twelve equivalent Sb1- atoms to form a mixture of face and corner-sharing PuSb12 cuboctahedra. There are six shorter (3.16 Å) and six longer (3.41 Å) Pu–Sb bond lengths. Sb1- is bonded in a 4-coordinate geometry to four equivalent Pu3+ atoms.
PuSb3 crystallizes in the tetragonal I4/mmm space group. The structure is three-dimensional. Pu3+ is bonded to twelve Sb1- atoms to form PuSb12 cuboctahedra that share corners with four equivalent PuSb12 cuboctahedra, edges with eight equivalent PuSb12 cuboctahedra, edges with sixteen equivalent SbPu4Sb8 cuboctahedra, faces with four equivalent PuSb12 cuboctahedra, and faces with eight equivalent SbPu4Sb8 cuboctahedra. There are four shorter (3.11 Å) and eight longer (3.42 Å) Pu–Sb bond lengths. There are two inequivalent Sb1- sites. In the first Sb1- site, Sb1- is bonded to four equivalent Pu3+ and eight Sb1- atoms to form distorted SbPu4Sb8 cuboctahedra that share corners with twelve equivalent SbPu4Sb8 cuboctahedra, edges with eight equivalent PuSb12 cuboctahedra, edges with eight equivalent SbPu4Sb8 cuboctahedra, faces with four equivalent PuSb12 cuboctahedra, and faces with ten equivalent SbPu4Sb8 cuboctahedra. There are four shorter (3.11 Å) and four longer (3.42 Å) Sb–Sb bond lengths. In the second Sb1- site, Sb1- is bonded in a square co-planar geometry to four equivalent Pu3+ and eight equivalent Sb1- atoms.