UGd2S5 crystallizes in the orthorhombic Pnma space group. U(1) is bonded in a 7-coordinate geometry to one S(2), one S(3), one S(4), and four equivalent S(1) atoms. Gd(1) is bonded in a 8-coordinate geometry to two equivalent S(1), two equivalent S(2), two equivalent S(3), and two equivalent S(4) atoms. There are four inequivalent S sites. In the first S site, S(1) is bonded to two equivalent U(1) and two equivalent Gd(1) atoms to form distorted SGd2U2 trigonal pyramids that share corners with two equivalent S(4)Gd4U square pyramids, corners with four equivalent S(3)Gd4U square pyramids, corners with two equivalent S(2)Gd4U trigonal bipyramids, corners with six equivalent S(1)Gd2U2 trigonal pyramids,  an edgeedge with one S(3)Gd4U square pyramid, edges with two equivalent S(4)Gd4U square pyramids, edges with two equivalent S(2)Gd4U trigonal bipyramids, and  an edgeedge with one S(1)Gd2U2 trigonal pyramid. In the second S site, S(2) is bonded to one U(1) and four equivalent Gd(1) atoms to form distorted SGd4U trigonal bipyramids that share  a cornercorner with one S(4)Gd4U square pyramid, corners with five equivalent S(3)Gd4U square pyramids, corners with four equivalent S(2)Gd4U trigonal bipyramids, corners with four equivalent S(1)Gd2U2 trigonal pyramids, edges with two equivalent S(3)Gd4U square pyramids, edges with four equivalent S(4)Gd4U square pyramids, and edges with four equivalent S(1)Gd2U2 trigonal pyramids. In the third S site, S(3) is bonded to one U(1) and four equivalent Gd(1) atoms to form SGd4U square pyramids that share corners with four equivalent S(4)Gd4U square pyramids, corners with five equivalent S(2)Gd4U trigonal bipyramids, corners with eight equivalent S(1)Gd2U2 trigonal pyramids,  an edgeedge with one S(4)Gd4U square pyramid, edges with two equivalent S(3)Gd4U square pyramids, edges with two equivalent S(2)Gd4U trigonal bipyramids, edges with two equivalent S(1)Gd2U2 trigonal pyramids, and  a faceface with one S(4)Gd4U square pyramid. In the fourth S site, S(4) is bonded to one U(1) and four equivalent Gd(1) atoms to form distorted SGd4U square pyramids that share corners with four equivalent S(3)Gd4U square pyramids, corners with four equivalent S(4)Gd4U square pyramids,  a cornercorner with one S(2)Gd4U trigonal bipyramid, corners with four equivalent S(1)Gd2U2 trigonal pyramids,  an edgeedge with one S(3)Gd4U square pyramid, edges with four equivalent S(2)Gd4U trigonal bipyramids, edges with four equivalent S(1)Gd2U2 trigonal pyramids, and  a faceface with one S(3)Gd4U square pyramid.
UGd2S5 crystallizes in the orthorhombic Pnma space group. U(1) is bonded in a 7-coordinate geometry to one S(2), one S(3), one S(4), and four equivalent S(1) atoms. The U(1)-S(2) bond length is 2.77 Å. The U(1)-S(3) bond length is 2.86 Å. The U(1)-S(4) bond length is 2.82 Å. There are two shorter (2.65 Å) and two longer (2.74 Å) U(1)-S(1) bond lengths. Gd(1) is bonded in a 8-coordinate geometry to two equivalent S(1), two equivalent S(2), two equivalent S(3), and two equivalent S(4) atoms. There is one shorter (2.82 Å) and one longer (2.85 Å) Gd(1)-S(1) bond length. There is one shorter (2.92 Å) and one longer (3.07 Å) Gd(1)-S(2) bond length. There is one shorter (2.90 Å) and one longer (2.93 Å) Gd(1)-S(3) bond length. There is one shorter (2.87 Å) and one longer (2.93 Å) Gd(1)-S(4) bond length. There are four inequivalent S sites. In the first S site, S(1) is bonded to two equivalent U(1) and two equivalent Gd(1) atoms to form distorted SGd2U2 trigonal pyramids that share corners with two equivalent S(4)Gd4U square pyramids, corners with four equivalent S(3)Gd4U square pyramids, corners with two equivalent S(2)Gd4U trigonal bipyramids, corners with six equivalent S(1)Gd2U2 trigonal pyramids,  an edgeedge with one S(3)Gd4U square pyramid, edges with two equivalent S(4)Gd4U square pyramids, edges with two equivalent S(2)Gd4U trigonal bipyramids, and  an edgeedge with one S(1)Gd2U2 trigonal pyramid. In the second S site, S(2) is bonded to one U(1) and four equivalent Gd(1) atoms to form distorted SGd4U trigonal bipyramids that share  a cornercorner with one S(4)Gd4U square pyramid, corners with five equivalent S(3)Gd4U square pyramids, corners with four equivalent S(2)Gd4U trigonal bipyramids, corners with four equivalent S(1)Gd2U2 trigonal pyramids, edges with two equivalent S(3)Gd4U square pyramids, edges with four equivalent S(4)Gd4U square pyramids, and edges with four equivalent S(1)Gd2U2 trigonal pyramids. In the third S site, S(3) is bonded to one U(1) and four equivalent Gd(1) atoms to form SGd4U square pyramids that share corners with four equivalent S(4)Gd4U square pyramids, corners with five equivalent S(2)Gd4U trigonal bipyramids, corners with eight equivalent S(1)Gd2U2 trigonal pyramids,  an edgeedge with one S(4)Gd4U square pyramid, edges with two equivalent S(3)Gd4U square pyramids, edges with two equivalent S(2)Gd4U trigonal bipyramids, edges with two equivalent S(1)Gd2U2 trigonal pyramids, and  a faceface with one S(4)Gd4U square pyramid. In the fourth S site, S(4) is bonded to one U(1) and four equivalent Gd(1) atoms to form distorted SGd4U square pyramids that share corners with four equivalent S(3)Gd4U square pyramids, corners with four equivalent S(4)Gd4U square pyramids,  a cornercorner with one S(2)Gd4U trigonal bipyramid, corners with four equivalent S(1)Gd2U2 trigonal pyramids,  an edgeedge with one S(3)Gd4U square pyramid, edges with four equivalent S(2)Gd4U trigonal bipyramids, edges with four equivalent S(1)Gd2U2 trigonal pyramids, and  a faceface with one S(3)Gd4U square pyramid.