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NpBr3 crystallizes in the hexagonal P6_3/m space group. The structure is three-dimensional. Np3+ is bonded in a 9-coordinate geometry to nine equivalent Br1- atoms. There are six shorter (3.06 Å) and three longer (3.15 Å) Np–Br bond lengths. Br1- is bonded in a trigonal non-coplanar geometry to three equivalent Np3+ atoms.
NpBr3 crystallizes in the orthorhombic Cmcm space group. The structure is two-dimensional and consists of two NpBr3 sheets oriented in the (0, 1, 0) direction. Np3+ is bonded in a 8-coordinate geometry to eight Br1- atoms. There are a spread of Np–Br bond distances ranging from 2.90–3.20 Å. There are two inequivalent Br1- sites. In the first Br1- site, Br1- is bonded in a distorted trigonal non-coplanar geometry to three equivalent Np3+ atoms. In the second Br1- site, Br1- is bonded in an L-shaped geometry to two equivalent Np3+ atoms.