Tb2Zr2O7 crystallizes in the cubic Fd-3m space group. Tb(1) is bonded in a body-centered cubic geometry to two equivalent O(1) and six equivalent O(2) atoms. Zr(1) is bonded to six equivalent O(2) atoms to form corner-sharing ZrO6 octahedra. The corner-sharing octahedral tilt angles are 54°. There are two inequivalent O sites. In the first O site, O(1) is bonded to four equivalent Tb(1) atoms to form OTb4 tetrahedra that share corners with four equivalent O(1)Tb4 tetrahedra, corners with twelve equivalent O(2)Tb2Zr2 tetrahedra, and edges with six equivalent O(2)Tb2Zr2 tetrahedra. In the second O site, O(2) is bonded to two equivalent Tb(1) and two equivalent Zr(1) atoms to form distorted OTb2Zr2 tetrahedra that share corners with two equivalent O(1)Tb4 tetrahedra, corners with twelve equivalent O(2)Tb2Zr2 tetrahedra,  an edgeedge with one O(1)Tb4 tetrahedra, and edges with four equivalent O(2)Tb2Zr2 tetrahedra.
Tb2Zr2O7 crystallizes in the cubic Fd-3m space group. Tb(1) is bonded in a body-centered cubic geometry to two equivalent O(1) and six equivalent O(2) atoms. Both Tb(1)-O(1) bond lengths are 2.30 Å. All Tb(1)-O(2) bond lengths are 2.53 Å. Zr(1) is bonded to six equivalent O(2) atoms to form corner-sharing ZrO6 octahedra. The corner-sharing octahedral tilt angles are 54°. All Zr(1)-O(2) bond lengths are 2.11 Å. There are two inequivalent O sites. In the first O site, O(1) is bonded to four equivalent Tb(1) atoms to form OTb4 tetrahedra that share corners with four equivalent O(1)Tb4 tetrahedra, corners with twelve equivalent O(2)Tb2Zr2 tetrahedra, and edges with six equivalent O(2)Tb2Zr2 tetrahedra. In the second O site, O(2) is bonded to two equivalent Tb(1) and two equivalent Zr(1) atoms to form distorted OTb2Zr2 tetrahedra that share corners with two equivalent O(1)Tb4 tetrahedra, corners with twelve equivalent O(2)Tb2Zr2 tetrahedra,  an edgeedge with one O(1)Tb4 tetrahedra, and edges with four equivalent O(2)Tb2Zr2 tetrahedra.