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TbAs3 crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Tb3+ is bonded to twelve equivalent As1- atoms to form a mixture of distorted face and corner-sharing TbAs12 cuboctahedra. There are six shorter (3.01 Å) and six longer (3.19 Å) Tb–As bond lengths. As1- is bonded in a 6-coordinate geometry to four equivalent Tb3+ and two equivalent As1- atoms. Both As–As bond lengths are 2.67 Å.
TbAs3 is Uranium Silicide structured and crystallizes in the cubic Pm-3m space group. The structure is three-dimensional. Tb3+ is bonded to twelve equivalent As1- atoms to form a mixture of face and corner-sharing TbAs12 cuboctahedra. All Tb–As bond lengths are 3.10 Å. As1- is bonded in a square co-planar geometry to four equivalent Tb3+ atoms.