U(CrAl10)2 crystallizes in the cubic Fd-3m space group. U(1) is bonded in a 16-coordinate geometry to four equivalent Al(1) and twelve equivalent Al(3) atoms. Cr(1) is bonded to six equivalent Al(2) and six equivalent Al(3) atoms to form CrAl12 cuboctahedra that share corners with six equivalent Cr(1)Al12 cuboctahedra, edges with eighteen equivalent Al(3)UAl10Cr cuboctahedra, and faces with six equivalent Al(3)UAl10Cr cuboctahedra. There are three inequivalent Al sites. In the first Al site, Al(1) is bonded in a distorted linear geometry to two equivalent U(1) and twelve equivalent Al(3) atoms. In the second Al site, Al(2) is bonded in a 12-coordinate geometry to two equivalent Cr(1), four equivalent Al(2), and six equivalent Al(3) atoms. In the third Al site, Al(3) is bonded to one U(1), one Cr(1), two equivalent Al(1), three equivalent Al(2), and five equivalent Al(3) atoms to form distorted AlUAl10Cr cuboctahedra that share corners with fifteen equivalent Al(3)UAl10Cr cuboctahedra, edges with two equivalent Al(3)UAl10Cr cuboctahedra, edges with three equivalent Cr(1)Al12 cuboctahedra,  a faceface with one Cr(1)Al12 cuboctahedra, and faces with fifteen equivalent Al(3)UAl10Cr cuboctahedra.
U(CrAl10)2 crystallizes in the cubic Fd-3m space group. U(1) is bonded in a 16-coordinate geometry to four equivalent Al(1) and twelve equivalent Al(3) atoms. All U(1)-Al(1) bond lengths are 3.11 Å. All U(1)-Al(3) bond lengths are 3.17 Å. Cr(1) is bonded to six equivalent Al(2) and six equivalent Al(3) atoms to form CrAl12 cuboctahedra that share corners with six equivalent Cr(1)Al12 cuboctahedra, edges with eighteen equivalent Al(3)UAl10Cr cuboctahedra, and faces with six equivalent Al(3)UAl10Cr cuboctahedra. All Cr(1)-Al(2) bond lengths are 2.54 Å. All Cr(1)-Al(3) bond lengths are 2.78 Å. There are three inequivalent Al sites. In the first Al site, Al(1) is bonded in a distorted linear geometry to two equivalent U(1) and twelve equivalent Al(3) atoms. All Al(1)-Al(3) bond lengths are 3.07 Å. In the second Al site, Al(2) is bonded in a 12-coordinate geometry to two equivalent Cr(1), four equivalent Al(2), and six equivalent Al(3) atoms. All Al(2)-Al(2) bond lengths are 2.77 Å. There are two shorter (2.70 Å) and four longer (2.82 Å) Al(2)-Al(3) bond lengths. In the third Al site, Al(3) is bonded to one U(1), one Cr(1), two equivalent Al(1), three equivalent Al(2), and five equivalent Al(3) atoms to form distorted AlUAl10Cr cuboctahedra that share corners with fifteen equivalent Al(3)UAl10Cr cuboctahedra, edges with two equivalent Al(3)UAl10Cr cuboctahedra, edges with three equivalent Cr(1)Al12 cuboctahedra,  a faceface with one Cr(1)Al12 cuboctahedra, and faces with fifteen equivalent Al(3)UAl10Cr cuboctahedra. There are a spread of Al(3)-Al(3) bond distances ranging from 2.68-2.90 Å.