U2S3 crystallizes in the orthorhombic Pnma space group. There are two inequivalent U sites. In the first U site, U(1) is bonded to one S(3), two equivalent S(2), and three equivalent S(1) atoms to form a mixture of corner and edge-sharing US6 octahedra. The corner-sharing octahedral tilt angles range from 6-71°. In the second U site, U(2) is bonded to one S(2), two equivalent S(1), and three equivalent S(3) atoms to form a mixture of corner and edge-sharing US6 octahedra. The corner-sharing octahedral tilt angles range from 6-71°. There are three inequivalent S sites. In the first S site, S(1) is bonded to two equivalent U(2) and three equivalent U(1) atoms to form SU5 square pyramids that share corners with seven equivalent S(3)U4 tetrahedra, edges with four equivalent S(1)U5 square pyramids, and  an edgeedge with one S(3)U4 tetrahedra. In the second S site, S(2) is bonded in a distorted T-shaped geometry to one U(2) and two equivalent U(1) atoms. In the third S site, S(3) is bonded to one U(1) and three equivalent U(2) atoms to form SU4 tetrahedra that share corners with seven equivalent S(1)U5 square pyramids, corners with two equivalent S(3)U4 tetrahedra,  an edgeedge with one S(1)U5 square pyramid, and edges with two equivalent S(3)U4 tetrahedra.
U2S3 crystallizes in the orthorhombic Pnma space group. There are two inequivalent U sites. In the first U site, U(1) is bonded to one S(3), two equivalent S(2), and three equivalent S(1) atoms to form a mixture of corner and edge-sharing US6 octahedra. The corner-sharing octahedral tilt angles range from 6-71°. The U(1)-S(3) bond length is 2.78 Å. Both U(1)-S(2) bond lengths are 2.67 Å. There is one shorter (2.76 Å) and two longer (2.78 Å) U(1)-S(1) bond lengths. In the second U site, U(2) is bonded to one S(2), two equivalent S(1), and three equivalent S(3) atoms to form a mixture of corner and edge-sharing US6 octahedra. The corner-sharing octahedral tilt angles range from 6-71°. The U(2)-S(2) bond length is 2.75 Å. Both U(2)-S(1) bond lengths are 2.78 Å. There are two shorter (2.73 Å) and one longer (2.75 Å) U(2)-S(3) bond length. There are three inequivalent S sites. In the first S site, S(1) is bonded to two equivalent U(2) and three equivalent U(1) atoms to form SU5 square pyramids that share corners with seven equivalent S(3)U4 tetrahedra, edges with four equivalent S(1)U5 square pyramids, and  an edgeedge with one S(3)U4 tetrahedra. In the second S site, S(2) is bonded in a distorted T-shaped geometry to one U(2) and two equivalent U(1) atoms. In the third S site, S(3) is bonded to one U(1) and three equivalent U(2) atoms to form SU4 tetrahedra that share corners with seven equivalent S(1)U5 square pyramids, corners with two equivalent S(3)U4 tetrahedra,  an edgeedge with one S(1)U5 square pyramid, and edges with two equivalent S(3)U4 tetrahedra.