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VBr3 crystallizes in the hexagonal P6_3/mmc space group. The structure is one-dimensional and consists of two VBr3 ribbons oriented in the (0, 0, 1) direction. V3+ is bonded to six equivalent Br1- atoms to form distorted face-sharing VBr6 pentagonal pyramids. All V–Br bond lengths are 2.56 Å. Br1- is bonded in an L-shaped geometry to two equivalent V3+ atoms.
VBr2 is trigonal omega structured and crystallizes in the trigonal P-3m1 space group. The structure is two-dimensional and consists of one VBr2 sheet oriented in the (0, 0, 1) direction. V2+ is bonded to six equivalent Br1- atoms to form edge-sharing VBr6 octahedra. All V–Br bond lengths are 2.65 Å. Br1- is bonded in a distorted T-shaped geometry to three equivalent V2+ atoms.