CsCrP2S7 crystallizes in the monoclinic C2 space group. Cs(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. Cr(1) is bonded to two equivalent S(1), two equivalent S(2), and two equivalent S(3) atoms to form CrS6 octahedra that share corners with two equivalent P(1)S4 tetrahedra and edges with two equivalent P(1)S4 tetrahedra. 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  a cornercorner with one Cr(1)S6 octahedra,  a cornercorner with one P(1)S4 tetrahedra, and  an edgeedge with one Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles are 64°. There are four inequivalent S sites. In the first S site, S(1) is bonded in a distorted L-shaped geometry to one Cs(1), one Cr(1), and one P(1) atom. In the second S site, S(2) is bonded in a distorted L-shaped geometry to one Cs(1), one Cr(1), and one P(1) atom. In the third S site, S(3) is bonded in a distorted bent 120 degrees geometry to one Cs(1), one Cr(1), and one P(1) atom. In the fourth S site, S(4) is bonded in a distorted water-like geometry to two equivalent Cs(1) and two equivalent P(1) atoms.
CsCrP2S7 crystallizes in the monoclinic C2 space group. Cs(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. Both Cs(1)-S(1) bond lengths are 3.80 Å. Both Cs(1)-S(2) bond lengths are 3.86 Å. Both Cs(1)-S(3) bond lengths are 3.63 Å. Both Cs(1)-S(4) bond lengths are 3.71 Å. Cr(1) is bonded to two equivalent S(1), two equivalent S(2), and two equivalent S(3) atoms to form CrS6 octahedra that share corners with two equivalent P(1)S4 tetrahedra and edges with two equivalent P(1)S4 tetrahedra. Both Cr(1)-S(1) bond lengths are 2.43 Å. Both Cr(1)-S(2) bond lengths are 2.43 Å. Both Cr(1)-S(3) bond lengths are 2.45 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  a cornercorner with one Cr(1)S6 octahedra,  a cornercorner with one P(1)S4 tetrahedra, and  an edgeedge with one Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles are 64°. The P(1)-S(1) bond length is 2.04 Å. The P(1)-S(2) bond length is 2.04 Å. The P(1)-S(3) bond length is 2.03 Å. The P(1)-S(4) bond length is 2.16 Å. There are four inequivalent S sites. In the first S site, S(1) is bonded in a distorted L-shaped geometry to one Cs(1), one Cr(1), and one P(1) atom. In the second S site, S(2) is bonded in a distorted L-shaped geometry to one Cs(1), one Cr(1), and one P(1) atom. In the third S site, S(3) is bonded in a distorted bent 120 degrees geometry to one Cs(1), one Cr(1), and one P(1) atom. In the fourth S site, S(4) is bonded in a distorted water-like geometry to two equivalent Cs(1) and two equivalent P(1) atoms.