TbCr2Si2 crystallizes in the tetragonal I4/mmm space group. Tb(1) is bonded in a 8-coordinate geometry to eight equivalent Si(1) atoms. Cr(1) is bonded to four equivalent Si(1) atoms to form a mixture of corner and edge-sharing CrSi4 tetrahedra. Si(1) is bonded in a 9-coordinate geometry to four equivalent Tb(1), four equivalent Cr(1), and one Si(1) atom.
TbCr2Si2 crystallizes in the tetragonal I4/mmm space group. Tb(1) is bonded in a 8-coordinate geometry to eight equivalent Si(1) atoms. All Tb(1)-Si(1) bond lengths are 3.00 Å. Cr(1) is bonded to four equivalent Si(1) atoms to form a mixture of corner and edge-sharing CrSi4 tetrahedra. All Cr(1)-Si(1) bond lengths are 2.41 Å. Si(1) is bonded in a 9-coordinate geometry to four equivalent Tb(1), four equivalent Cr(1), and one Si(1) atom. The Si(1)-Si(1) bond length is 2.48 Å.