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PuI2 is Rutile structured and crystallizes in the tetragonal P4_2/mnm space group. The structure is three-dimensional. Pu is bonded to six equivalent I atoms to form a mixture of corner and edge-sharing PuI6 octahedra. The corner-sharing octahedral tilt angles are 45°. There are four shorter (3.21 Å) and two longer (3.25 Å) Pu–I bond lengths. I is bonded in a distorted T-shaped geometry to three equivalent Pu atoms.
Pu3I is Uranium Silicide-like structured and crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Pu is bonded in a distorted see-saw-like geometry to four equivalent I atoms. There are two shorter (3.32 Å) and two longer (3.41 Å) Pu–I bond lengths. I is bonded to twelve equivalent Pu atoms to form a mixture of corner and face-sharing IPu12 cuboctahedra.