U5SiS4 is Caswellsilverite-like structured and crystallizes in the tetragonal I4/m space group. There are three inequivalent U sites. In the first U site, U(1) is bonded to one Si(1) and five equivalent S(1) atoms to form USiS5 octahedra that share  a cornercorner with one U(2)Si2S4 octahedra; corners with five U(1,1)SiS5 octahedra; edges with three equivalent U(2)Si2S4 octahedra; and edges with nine U(1,1)SiS5 octahedra. The corner-sharing octahedral tilt angles range from 0-2°. In the second U site, U(2) is bonded to two equivalent Si(1) and four equivalent S(1) atoms to form USi2S4 octahedra that share corners with two equivalent U(2)Si2S4 octahedra; corners with four U(1,1)SiS5 octahedra; and edges with twelve U(1,1)SiS5 octahedra. The corner-sharing octahedral tilt angles range from 0-2°. In the third U site, U(1) is bonded to one Si(1) and five equivalent S(1) atoms to form USiS5 octahedra that share  a cornercorner with one U(2)Si2S4 octahedra; corners with five U(1,1)SiS5 octahedra; edges with three equivalent U(2)Si2S4 octahedra; and edges with nine U(1,1)SiS5 octahedra. The corner-sharing octahedral tilt angles range from 0-2°. Si(1) is bonded to two equivalent U(2) and four U(1,1) atoms to form SiU6 octahedra that share corners with two equivalent Si(1)U6 octahedra, corners with four equivalent S(1)U6 octahedra, and edges with twelve equivalent S(1)U6 octahedra. The corner-sharing octahedra are not tilted. S(1) is bonded to one U(2) and five U(1,1) atoms to form SU6 octahedra that share  a cornercorner with one Si(1)U6 octahedra, corners with five equivalent S(1)U6 octahedra, edges with three equivalent Si(1)U6 octahedra, and edges with nine equivalent S(1)U6 octahedra. The corner-sharing octahedral tilt angles range from 0-2°.
U5SiS4 is Caswellsilverite-like structured and crystallizes in the tetragonal I4/m space group. There are three inequivalent U sites. In the first U site, U(1) is bonded to one Si(1) and five equivalent S(1) atoms to form USiS5 octahedra that share  a cornercorner with one U(2)Si2S4 octahedra; corners with five U(1,1)SiS5 octahedra; edges with three equivalent U(2)Si2S4 octahedra; and edges with nine U(1,1)SiS5 octahedra. The corner-sharing octahedral tilt angles range from 0-2°. The U(1)-Si(1) bond length is 2.80 Å. There are two shorter (2.74 Å) and three longer (2.76 Å) U(1)-S(1) bond lengths. In the second U site, U(2) is bonded to two equivalent Si(1) and four equivalent S(1) atoms to form USi2S4 octahedra that share corners with two equivalent U(2)Si2S4 octahedra; corners with four U(1,1)SiS5 octahedra; and edges with twelve U(1,1)SiS5 octahedra. The corner-sharing octahedral tilt angles range from 0-2°. Both U(2)-Si(1) bond lengths are 2.76 Å. All U(2)-S(1) bond lengths are 2.76 Å. In the third U site, U(1) is bonded to one Si(1) and five equivalent S(1) atoms to form USiS5 octahedra that share  a cornercorner with one U(2)Si2S4 octahedra; corners with five U(1,1)SiS5 octahedra; edges with three equivalent U(2)Si2S4 octahedra; and edges with nine U(1,1)SiS5 octahedra. The corner-sharing octahedral tilt angles range from 0-2°. The U(1)-Si(1) bond length is 2.80 Å. There are two shorter (2.74 Å) and three longer (2.76 Å) U(1)-S(1) bond lengths. Si(1) is bonded to two equivalent U(2) and four U(1,1) atoms to form SiU6 octahedra that share corners with two equivalent Si(1)U6 octahedra, corners with four equivalent S(1)U6 octahedra, and edges with twelve equivalent S(1)U6 octahedra. The corner-sharing octahedra are not tilted. S(1) is bonded to one U(2) and five U(1,1) atoms to form SU6 octahedra that share  a cornercorner with one Si(1)U6 octahedra, corners with five equivalent S(1)U6 octahedra, edges with three equivalent Si(1)U6 octahedra, and edges with nine equivalent S(1)U6 octahedra. The corner-sharing octahedral tilt angles range from 0-2°.