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TbSb2 is trigonal omega structured and crystallizes in the orthorhombic C222 space group. The structure is two-dimensional and consists of one TbSb2 sheet oriented in the (0, 0, 1) direction. Tb3+ is bonded in a 4-coordinate geometry to four equivalent Sb+1.50- atoms. All Tb–Sb bond lengths are 3.07 Å. Sb+1.50- is bonded in a 2-coordinate geometry to two equivalent Tb3+ atoms.
TbSb2Sb crystallizes in the orthorhombic Cmmm space group. The structure is two-dimensional and consists of two antimony molecules and one TbSb2 sheet oriented in the (0, 0, 1) direction. In the TbSb2 sheet, Tb3+ is bonded in a distorted rectangular see-saw-like geometry to four equivalent Sb1- atoms. All Tb–Sb bond lengths are 3.00 Å. Sb1- is bonded in a distorted linear geometry to two equivalent Tb3+ atoms.