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NdI2 crystallizes in the tetragonal I4/mmm space group. The structure is two-dimensional and consists of two NdI2 sheets oriented in the (0, 0, 1) direction. Nd2+ is bonded in a body-centered cubic geometry to eight equivalent I1- atoms. All Nd–I bond lengths are 3.33 Å. I1- is bonded in a 4-coordinate geometry to four equivalent Nd2+ atoms.
NdI3 crystallizes in the hexagonal P6_3/mmc space group. The structure is one-dimensional and consists of two NdI3 ribbons oriented in the (0, 0, 1) direction. Nd3+ is bonded to six equivalent I1- atoms to form distorted face-sharing NdI6 pentagonal pyramids. All Nd–I bond lengths are 3.15 Å. I1- is bonded in an L-shaped geometry to two equivalent Nd3+ atoms.