U3(PS4)4 crystallizes in the tetragonal I-4c2 space group. There are three inequivalent U sites. In the first U site, U(1) is bonded to four equivalent S(1) and four equivalent S(4) atoms to form distorted US8 hexagonal bipyramids that share edges with four equivalent P(1)S4 tetrahedra. In the second U site, U(2) is bonded to four equivalent S(2) and four equivalent S(3) atoms to form distorted US8 hexagonal bipyramids that share edges with four equivalent P(1)S4 tetrahedra. In the third U site, U(3) is bonded in a 8-coordinate geometry to four equivalent S(1) and four equivalent S(3) atoms. P(1) is bonded to one S(1), one S(2), one S(3), and one S(4) atom to form PS4 tetrahedra that share  an edgeedge with one U(1)S8 hexagonal bipyramid and  an edgeedge with one U(2)S8 hexagonal bipyramid. There are four inequivalent S sites. In the first S site, S(3) is bonded in a distorted T-shaped geometry to one U(2), one U(3), and one P(1) atom. In the second S site, S(4) is bonded in a water-like geometry to one U(1) and one P(1) atom. In the third S site, S(1) is bonded in a distorted T-shaped geometry to one U(1), one U(3), and one P(1) atom. In the fourth S site, S(2) is bonded in an L-shaped geometry to one U(2) and one P(1) atom.
U3(PS4)4 crystallizes in the tetragonal I-4c2 space group. There are three inequivalent U sites. In the first U site, U(1) is bonded to four equivalent S(1) and four equivalent S(4) atoms to form distorted US8 hexagonal bipyramids that share edges with four equivalent P(1)S4 tetrahedra. All U(1)-S(1) bond lengths are 3.01 Å. All U(1)-S(4) bond lengths are 2.77 Å. In the second U site, U(2) is bonded to four equivalent S(2) and four equivalent S(3) atoms to form distorted US8 hexagonal bipyramids that share edges with four equivalent P(1)S4 tetrahedra. All U(2)-S(2) bond lengths are 2.81 Å. All U(2)-S(3) bond lengths are 2.92 Å. In the third U site, U(3) is bonded in a 8-coordinate geometry to four equivalent S(1) and four equivalent S(3) atoms. All U(3)-S(1) bond lengths are 2.85 Å. All U(3)-S(3) bond lengths are 2.94 Å. P(1) is bonded to one S(1), one S(2), one S(3), and one S(4) atom to form PS4 tetrahedra that share  an edgeedge with one U(1)S8 hexagonal bipyramid and  an edgeedge with one U(2)S8 hexagonal bipyramid. The P(1)-S(1) bond length is 2.07 Å. The P(1)-S(2) bond length is 2.03 Å. The P(1)-S(3) bond length is 2.08 Å. The P(1)-S(4) bond length is 2.05 Å. There are four inequivalent S sites. In the first S site, S(3) is bonded in a distorted T-shaped geometry to one U(2), one U(3), and one P(1) atom. In the second S site, S(4) is bonded in a water-like geometry to one U(1) and one P(1) atom. In the third S site, S(1) is bonded in a distorted T-shaped geometry to one U(1), one U(3), and one P(1) atom. In the fourth S site, S(2) is bonded in an L-shaped geometry to one U(2) and one P(1) atom.