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Ce4As3 crystallizes in the cubic I-43d space group. The structure is three-dimensional. Ce is bonded in a 6-coordinate geometry to six equivalent As atoms. There are three shorter (2.96 Å) and three longer (3.21 Å) Ce–As bond lengths. As is bonded to eight equivalent Ce atoms to form a mixture of distorted corner, edge, and face-sharing AsCe8 hexagonal bipyramids.
CeAs is Halite, Rock Salt structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Ce3+ is bonded to six equivalent As3- atoms to form a mixture of corner and edge-sharing CeAs6 octahedra. The corner-sharing octahedral tilt angles are 0°. All Ce–As bond lengths are 2.99 Å. As3- is bonded to six equivalent Ce3+ atoms to form a mixture of corner and edge-sharing AsCe6 octahedra. The corner-sharing octahedral tilt angles are 0°.
CeAs2 is Cotunnite structured and crystallizes in the monoclinic P2_1/c space group. The structure is three-dimensional. Ce4+ is bonded in a 9-coordinate geometry to nine As2- atoms. There are a spread of Ce–As bond distances ranging from 2.98–3.16 Å. There are two inequivalent As2- sites. In the first As2- site, As2- is bonded in a 5-coordinate geometry to five equivalent Ce4+ and two equivalent As2- atoms. There are one shorter (3.04 Å) and one longer (3.07 Å) As–As bond lengths. In the second As2- site, As2- is bonded in a 8-coordinate geometry to four equivalent Ce4+ and four As2- atoms. There are one shorter (2.66 Å) and one longer (2.69 Å) As–As bond lengths.