U(CrAl10)2 crystallizes in the cubic Fd-3m space group. U(1) is bonded in a 16-coordinate geometry to four equivalent Cr(1) and twelve equivalent Al(2) atoms. Cr(1) is bonded in a 14-coordinate geometry to two equivalent U(1) and twelve equivalent Al(2) atoms. There are three inequivalent Al sites. In the first Al site, Al(1) is bonded to two equivalent Al(3), four equivalent Al(1), and six equivalent Al(2) atoms to form distorted AlAl12 cuboctahedra that share corners with two equivalent Al(1)Al12 cuboctahedra, corners with sixteen equivalent Al(2)UAl9Cr2 cuboctahedra, edges with two equivalent Al(3)Al12 cuboctahedra, faces with two equivalent Al(3)Al12 cuboctahedra, faces with nine equivalent Al(1)Al12 cuboctahedra, and faces with fourteen equivalent Al(2)UAl9Cr2 cuboctahedra. In the second Al site, Al(3) is bonded to six equivalent Al(1) and six equivalent Al(2) atoms to form AlAl12 cuboctahedra that share corners with six equivalent Al(3)Al12 cuboctahedra, edges with six equivalent Al(1)Al12 cuboctahedra, edges with eighteen equivalent Al(2)UAl9Cr2 cuboctahedra, faces with six equivalent Al(1)Al12 cuboctahedra, and faces with six equivalent Al(2)UAl9Cr2 cuboctahedra. In the third Al site, Al(2) is bonded to one U(1), two equivalent Cr(1), one Al(3), three equivalent Al(1), and five equivalent Al(2) atoms to form distorted AlUAl9Cr2 cuboctahedra that share corners with eight equivalent Al(1)Al12 cuboctahedra, corners with fifteen equivalent Al(2)UAl9Cr2 cuboctahedra, edges with two equivalent Al(2)UAl9Cr2 cuboctahedra, edges with three equivalent Al(3)Al12 cuboctahedra,  a faceface with one Al(3)Al12 cuboctahedra, faces with seven equivalent Al(1)Al12 cuboctahedra, and faces with fifteen equivalent Al(2)UAl9Cr2 cuboctahedra.
U(CrAl10)2 crystallizes in the cubic Fd-3m space group. U(1) is bonded in a 16-coordinate geometry to four equivalent Cr(1) and twelve equivalent Al(2) atoms. All U(1)-Cr(1) bond lengths are 3.17 Å. All U(1)-Al(2) bond lengths are 3.16 Å. Cr(1) is bonded in a 14-coordinate geometry to two equivalent U(1) and twelve equivalent Al(2) atoms. All Cr(1)-Al(2) bond lengths are 3.08 Å. There are three inequivalent Al sites. In the first Al site, Al(1) is bonded to two equivalent Al(3), four equivalent Al(1), and six equivalent Al(2) atoms to form distorted AlAl12 cuboctahedra that share corners with two equivalent Al(1)Al12 cuboctahedra, corners with sixteen equivalent Al(2)UAl9Cr2 cuboctahedra, edges with two equivalent Al(3)Al12 cuboctahedra, faces with two equivalent Al(3)Al12 cuboctahedra, faces with nine equivalent Al(1)Al12 cuboctahedra, and faces with fourteen equivalent Al(2)UAl9Cr2 cuboctahedra. Both Al(1)-Al(3) bond lengths are 2.59 Å. All Al(1)-Al(1) bond lengths are 2.84 Å. There are two shorter (2.77 Å) and four longer (2.93 Å) Al(1)-Al(2) bond lengths. In the second Al site, Al(3) is bonded to six equivalent Al(1) and six equivalent Al(2) atoms to form AlAl12 cuboctahedra that share corners with six equivalent Al(3)Al12 cuboctahedra, edges with six equivalent Al(1)Al12 cuboctahedra, edges with eighteen equivalent Al(2)UAl9Cr2 cuboctahedra, faces with six equivalent Al(1)Al12 cuboctahedra, and faces with six equivalent Al(2)UAl9Cr2 cuboctahedra. All Al(3)-Al(2) bond lengths are 2.91 Å. In the third Al site, Al(2) is bonded to one U(1), two equivalent Cr(1), one Al(3), three equivalent Al(1), and five equivalent Al(2) atoms to form distorted AlUAl9Cr2 cuboctahedra that share corners with eight equivalent Al(1)Al12 cuboctahedra, corners with fifteen equivalent Al(2)UAl9Cr2 cuboctahedra, edges with two equivalent Al(2)UAl9Cr2 cuboctahedra, edges with three equivalent Al(3)Al12 cuboctahedra,  a faceface with one Al(3)Al12 cuboctahedra, faces with seven equivalent Al(1)Al12 cuboctahedra, and faces with fifteen equivalent Al(2)UAl9Cr2 cuboctahedra. There are a spread of Al(2)-Al(2) bond distances ranging from 2.63-3.02 Å.