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CrBr2 crystallizes in the monoclinic C2/m space group. The structure is two-dimensional and consists of one CrBr2 sheet oriented in the (0, 0, 1) direction. Cr2+ is bonded to six equivalent Br1- atoms to form edge-sharing CrBr6 octahedra. There are four shorter (2.55 Å) and two longer (3.20 Å) Cr–Br bond lengths. Br1- is bonded in a 2-coordinate geometry to three equivalent Cr2+ atoms.
CrBr2 is zeta iron carbide structured and crystallizes in the tetragonal P4_2/mnm space group. The structure is three-dimensional. Cr2+ is bonded to six equivalent Br1- atoms to form a mixture of corner and edge-sharing CrBr6 octahedra. The corner-sharing octahedral tilt angles are 47°. There are four shorter (2.55 Å) and two longer (3.03 Å) Cr–Br bond lengths. Br1- is bonded in a 3-coordinate geometry to three equivalent Cr2+ atoms.