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I2Cr crystallizes in the monoclinic C2/m space group. The structure is two-dimensional and consists of one I2Cr sheet oriented in the (0, 0, 1) direction. Cr2+ is bonded to six equivalent I1- atoms to form edge-sharing CrI6 octahedra. There are four shorter (2.74 Å) and two longer (3.37 Å) Cr–I bond lengths. I1- is bonded in a 3-coordinate geometry to three equivalent Cr2+ atoms.
I2Cr is Molybdenite structured and crystallizes in the orthorhombic Cmc2_1 space group. The structure is two-dimensional and consists of two I2Cr sheets oriented in the (0, 0, 1) direction. Cr2+ is bonded to five I1- atoms to form a mixture of distorted corner and edge-sharing CrI5 square pyramids. There are four shorter (2.73 Å) and one longer (3.48 Å) Cr–I bond lengths. There are two inequivalent I1- sites. In the first I1- site, I1- is bonded in an L-shaped geometry to two equivalent Cr2+ atoms. In the second I1- site, I1- is bonded in a 2-coordinate geometry to three equivalent Cr2+ atoms.
I2Cr is trigonal omega-like structured and crystallizes in the orthorhombic Cmc2_1 space group. The structure is two-dimensional and consists of two I2Cr sheets oriented in the (0, 0, 1) direction. Cr2+ is bonded to six I1- atoms to form edge-sharing CrI6 octahedra. There are a spread of Cr–I bond distances ranging from 2.87–2.90 Å. There are two inequivalent I1- sites. In the first I1- site, I1- is bonded in a distorted T-shaped geometry to three equivalent Cr2+ atoms. In the second I1- site, I1- is bonded in a distorted T-shaped geometry to three equivalent Cr2+ atoms.