Al2TiO5 crystallizes in the orthorhombic Cmcm space group. Ti(1) is bonded in a 6-coordinate geometry to two equivalent O(1), two equivalent O(2), and two equivalent O(3) atoms. Al(1) is bonded to one O(3), two equivalent O(2), and three equivalent O(1) atoms to form a mixture of distorted edge and corner-sharing AlO6 octahedra. The corner-sharing octahedral tilt angles range from 28-50°. There are three inequivalent O sites. In the first O site, O(1) is bonded to one Ti(1) and three equivalent Al(1) atoms to form distorted OTiAl3 trigonal pyramids that share  a cornercorner with one O(3)Ti2Al2 trigonal pyramid, corners with three equivalent O(1)TiAl3 trigonal pyramids, edges with two equivalent O(3)Ti2Al2 trigonal pyramids, and edges with two equivalent O(1)TiAl3 trigonal pyramids. In the second O site, O(2) is bonded in a distorted T-shaped geometry to one Ti(1) and two equivalent Al(1) atoms. In the third O site, O(3) is bonded to two equivalent Ti(1) and two equivalent Al(1) atoms to form distorted OTi2Al2 trigonal pyramids that share corners with two equivalent O(3)Ti2Al2 trigonal pyramids, corners with two equivalent O(1)TiAl3 trigonal pyramids, and edges with four equivalent O(1)TiAl3 trigonal pyramids.
Al2TiO5 crystallizes in the orthorhombic Cmcm space group. Ti(1) is bonded in a 6-coordinate geometry to two equivalent O(1), two equivalent O(2), and two equivalent O(3) atoms. Both Ti(1)-O(1) bond lengths are 2.14 Å. Both Ti(1)-O(2) bond lengths are 1.84 Å. Both Ti(1)-O(3) bond lengths are 1.95 Å. Al(1) is bonded to one O(3), two equivalent O(2), and three equivalent O(1) atoms to form a mixture of distorted edge and corner-sharing AlO6 octahedra. The corner-sharing octahedral tilt angles range from 28-50°. The Al(1)-O(3) bond length is 2.07 Å. There is one shorter (1.83 Å) and one longer (1.89 Å) Al(1)-O(2) bond length. There are two shorter (1.85 Å) and one longer (1.99 Å) Al(1)-O(1) bond length. There are three inequivalent O sites. In the first O site, O(1) is bonded to one Ti(1) and three equivalent Al(1) atoms to form distorted OTiAl3 trigonal pyramids that share  a cornercorner with one O(3)Ti2Al2 trigonal pyramid, corners with three equivalent O(1)TiAl3 trigonal pyramids, edges with two equivalent O(3)Ti2Al2 trigonal pyramids, and edges with two equivalent O(1)TiAl3 trigonal pyramids. In the second O site, O(2) is bonded in a distorted T-shaped geometry to one Ti(1) and two equivalent Al(1) atoms. In the third O site, O(3) is bonded to two equivalent Ti(1) and two equivalent Al(1) atoms to form distorted OTi2Al2 trigonal pyramids that share corners with two equivalent O(3)Ti2Al2 trigonal pyramids, corners with two equivalent O(1)TiAl3 trigonal pyramids, and edges with four equivalent O(1)TiAl3 trigonal pyramids.