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TmI2 is trigonal omega structured and crystallizes in the trigonal P-3m1 space group. The structure is two-dimensional and consists of one TmI2 sheet oriented in the (0, 0, 1) direction. Tm is bonded to six equivalent I atoms to form edge-sharing TmI6 octahedra. All Tm–I bond lengths are 3.04 Å. I is bonded in a distorted T-shaped geometry to three equivalent Tm atoms.
TmI3 crystallizes in the hexagonal P6_3/mmc space group. The structure is one-dimensional and consists of two TmI3 ribbons oriented in the (0, 0, 1) direction. Tm3+ is bonded to six equivalent I1- atoms to form distorted face-sharing TmI6 pentagonal pyramids. All Tm–I bond lengths are 3.03 Å. I1- is bonded in an L-shaped geometry to two equivalent Tm3+ atoms.