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Ac3I crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Ac is bonded in a distorted see-saw-like geometry to four equivalent I atoms. There are two shorter (3.77 Å) and two longer (3.96 Å) Ac–I bond lengths. I is bonded to twelve equivalent Ac atoms to form a mixture of corner and face-sharing IAc12 cuboctahedra.
Ac3I is Uranium Silicide-like structured and crystallizes in the tetragonal I4/mmm space group. The structure is three-dimensional. there are two inequivalent Ac sites. In the first Ac site, Ac is bonded to four equivalent I atoms to form a mixture of distorted corner and edge-sharing AcI4 cuboctahedra. All Ac–I bond lengths are 3.93 Å. In the second Ac site, Ac is bonded in a square co-planar geometry to four equivalent I atoms. All Ac–I bond lengths are 3.85 Å. I is bonded to twelve Ac atoms to form a mixture of corner, edge, and face-sharing IAc12 cuboctahedra.