TaCr3(AgS4)2 crystallizes in the monoclinic P2_1/m space group. Ta(1) is bonded to one S(3), one S(8), two equivalent S(1), and two equivalent S(6) atoms to form distorted TaS6 octahedra that share corners with three equivalent Cr(1)S6 octahedra, edges with two equivalent Ta(1)S6 octahedra, and edges with two equivalent Cr(2)S6 octahedra. The corner-sharing octahedral tilt angles range from 55-57°. There are three inequivalent Cr sites. In the first Cr site, Cr(1) is bonded to one S(5), two equivalent S(7), and three equivalent S(3) atoms to form CrS6 octahedra that share corners with three equivalent Ta(1)S6 octahedra, edges with two equivalent Cr(3)S6 octahedra, and edges with four equivalent Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 55-57°. In the second Cr site, Cr(2) is bonded to one S(6), two equivalent S(8), and three equivalent S(4) atoms to form CrS6 octahedra that share corners with three equivalent Cr(3)S6 octahedra, edges with two equivalent Ta(1)S6 octahedra, and edges with four equivalent Cr(2)S6 octahedra. The corner-sharing octahedral tilt angles range from 53-58°. In the third Cr site, Cr(3) is bonded to one S(4), one S(7), two equivalent S(2), and two equivalent S(5) atoms to form a mixture of corner and edge-sharing CrS6 octahedra. The corner-sharing octahedral tilt angles range from 53-58°. There are two inequivalent Ag sites. In the first Ag site, Ag(1) is bonded in a 7-coordinate geometry to two equivalent S(5), two equivalent S(8), and three equivalent S(1) atoms. In the second Ag site, Ag(2) is bonded in a 7-coordinate geometry to two equivalent S(6), two equivalent S(7), and three equivalent S(2) atoms. There are eight inequivalent S sites. In the first S site, S(1) is bonded in a 5-coordinate geometry to two equivalent Ta(1) and three equivalent Ag(1) atoms. In the second S site, S(2) is bonded to two equivalent Cr(3) and three equivalent Ag(2) atoms to form distorted SCr2Ag3 square pyramids that share corners with two equivalent S(7)Cr3Ag2 square pyramids, corners with two equivalent S(5)Cr3Ag2 trigonal bipyramids, corners with four equivalent S(6)Ta2CrAg2 trigonal bipyramids, edges with three equivalent S(7)Cr3Ag2 square pyramids, edges with four equivalent S(2)Cr2Ag3 square pyramids,  an edgeedge with one S(5)Cr3Ag2 trigonal bipyramid, and  an edgeedge with one S(6)Ta2CrAg2 trigonal bipyramid. In the third S site, S(3) is bonded in a rectangular see-saw-like geometry to one Ta(1) and three equivalent Cr(1) atoms. In the fourth S site, S(4) is bonded in a rectangular see-saw-like geometry to one Cr(3) and three equivalent Cr(2) atoms. In the fifth S site, S(5) is bonded to one Cr(1), two equivalent Cr(3), and two equivalent Ag(1) atoms to form distorted SCr3Ag2 trigonal bipyramids that share corners with two equivalent S(2)Cr2Ag3 square pyramids, corners with two equivalent S(8)TaCr2Ag2 square pyramids,  an edgeedge with one S(2)Cr2Ag3 square pyramid,  an edgeedge with one S(8)TaCr2Ag2 square pyramid, edges with two equivalent S(7)Cr3Ag2 square pyramids, and edges with two equivalent S(5)Cr3Ag2 trigonal bipyramids. In the sixth S site, S(6) is bonded to two equivalent Ta(1), one Cr(2), and two equivalent Ag(2) atoms to form distorted STa2CrAg2 trigonal bipyramids that share corners with two equivalent S(7)Cr3Ag2 square pyramids, corners with four equivalent S(2)Cr2Ag3 square pyramids,  an edgeedge with one S(2)Cr2Ag3 square pyramid,  an edgeedge with one S(7)Cr3Ag2 square pyramid, edges with two equivalent S(8)TaCr2Ag2 square pyramids, and edges with two equivalent S(6)Ta2CrAg2 trigonal bipyramids. In the seventh S site, S(7) is bonded to one Cr(3), two equivalent Cr(1), and two equivalent Ag(2) atoms to form distorted SCr3Ag2 square pyramids that share corners with two equivalent S(2)Cr2Ag3 square pyramids, corners with two equivalent S(6)Ta2CrAg2 trigonal bipyramids, edges with two equivalent S(7)Cr3Ag2 square pyramids, edges with three equivalent S(2)Cr2Ag3 square pyramids,  an edgeedge with one S(6)Ta2CrAg2 trigonal bipyramid, and edges with two equivalent S(5)Cr3Ag2 trigonal bipyramids. In the eighth S site, S(8) is bonded to one Ta(1), two equivalent Cr(2), and two equivalent Ag(1) atoms to form distorted STaCr2Ag2 square pyramids that share corners with two equivalent S(5)Cr3Ag2 trigonal bipyramids, edges with two equivalent S(8)TaCr2Ag2 square pyramids,  an edgeedge with one S(5)Cr3Ag2 trigonal bipyramid, and edges with two equivalent S(6)Ta2CrAg2 trigonal bipyramids.
TaCr3(AgS4)2 crystallizes in the monoclinic P2_1/m space group. Ta(1) is bonded to one S(3), one S(8), two equivalent S(1), and two equivalent S(6) atoms to form distorted TaS6 octahedra that share corners with three equivalent Cr(1)S6 octahedra, edges with two equivalent Ta(1)S6 octahedra, and edges with two equivalent Cr(2)S6 octahedra. The corner-sharing octahedral tilt angles range from 55-57°. The Ta(1)-S(3) bond length is 2.44 Å. The Ta(1)-S(8) bond length is 2.60 Å. Both Ta(1)-S(1) bond lengths are 2.44 Å. Both Ta(1)-S(6) bond lengths are 2.47 Å. There are three inequivalent Cr sites. In the first Cr site, Cr(1) is bonded to one S(5), two equivalent S(7), and three equivalent S(3) atoms to form CrS6 octahedra that share corners with three equivalent Ta(1)S6 octahedra, edges with two equivalent Cr(3)S6 octahedra, and edges with four equivalent Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 55-57°. The Cr(1)-S(5) bond length is 2.37 Å. Both Cr(1)-S(7) bond lengths are 2.33 Å. There are two shorter (2.50 Å) and one longer (2.64 Å) Cr(1)-S(3) bond length. In the second Cr site, Cr(2) is bonded to one S(6), two equivalent S(8), and three equivalent S(4) atoms to form CrS6 octahedra that share corners with three equivalent Cr(3)S6 octahedra, edges with two equivalent Ta(1)S6 octahedra, and edges with four equivalent Cr(2)S6 octahedra. The corner-sharing octahedral tilt angles range from 53-58°. The Cr(2)-S(6) bond length is 2.56 Å. Both Cr(2)-S(8) bond lengths are 2.39 Å. There are two shorter (2.41 Å) and one longer (2.44 Å) Cr(2)-S(4) bond length. In the third Cr site, Cr(3) is bonded to one S(4), one S(7), two equivalent S(2), and two equivalent S(5) atoms to form a mixture of corner and edge-sharing CrS6 octahedra. The corner-sharing octahedral tilt angles range from 53-58°. The Cr(3)-S(4) bond length is 2.62 Å. The Cr(3)-S(7) bond length is 2.41 Å. Both Cr(3)-S(2) bond lengths are 2.36 Å. Both Cr(3)-S(5) bond lengths are 2.43 Å. There are two inequivalent Ag sites. In the first Ag site, Ag(1) is bonded in a 7-coordinate geometry to two equivalent S(5), two equivalent S(8), and three equivalent S(1) atoms. Both Ag(1)-S(5) bond lengths are 2.70 Å. Both Ag(1)-S(8) bond lengths are 2.75 Å. There is one shorter (2.85 Å) and two longer (2.87 Å) Ag(1)-S(1) bond lengths. In the second Ag site, Ag(2) is bonded in a 7-coordinate geometry to two equivalent S(6), two equivalent S(7), and three equivalent S(2) atoms. Both Ag(2)-S(6) bond lengths are 2.90 Å. Both Ag(2)-S(7) bond lengths are 2.79 Å. There is one shorter (2.64 Å) and two longer (2.72 Å) Ag(2)-S(2) bond lengths. There are eight inequivalent S sites. In the first S site, S(1) is bonded in a 5-coordinate geometry to two equivalent Ta(1) and three equivalent Ag(1) atoms. In the second S site, S(2) is bonded to two equivalent Cr(3) and three equivalent Ag(2) atoms to form distorted SCr2Ag3 square pyramids that share corners with two equivalent S(7)Cr3Ag2 square pyramids, corners with two equivalent S(5)Cr3Ag2 trigonal bipyramids, corners with four equivalent S(6)Ta2CrAg2 trigonal bipyramids, edges with three equivalent S(7)Cr3Ag2 square pyramids, edges with four equivalent S(2)Cr2Ag3 square pyramids,  an edgeedge with one S(5)Cr3Ag2 trigonal bipyramid, and  an edgeedge with one S(6)Ta2CrAg2 trigonal bipyramid. In the third S site, S(3) is bonded in a rectangular see-saw-like geometry to one Ta(1) and three equivalent Cr(1) atoms. In the fourth S site, S(4) is bonded in a rectangular see-saw-like geometry to one Cr(3) and three equivalent Cr(2) atoms. In the fifth S site, S(5) is bonded to one Cr(1), two equivalent Cr(3), and two equivalent Ag(1) atoms to form distorted SCr3Ag2 trigonal bipyramids that share corners with two equivalent S(2)Cr2Ag3 square pyramids, corners with two equivalent S(8)TaCr2Ag2 square pyramids,  an edgeedge with one S(2)Cr2Ag3 square pyramid,  an edgeedge with one S(8)TaCr2Ag2 square pyramid, edges with two equivalent S(7)Cr3Ag2 square pyramids, and edges with two equivalent S(5)Cr3Ag2 trigonal bipyramids. In the sixth S site, S(6) is bonded to two equivalent Ta(1), one Cr(2), and two equivalent Ag(2) atoms to form distorted STa2CrAg2 trigonal bipyramids that share corners with two equivalent S(7)Cr3Ag2 square pyramids, corners with four equivalent S(2)Cr2Ag3 square pyramids,  an edgeedge with one S(2)Cr2Ag3 square pyramid,  an edgeedge with one S(7)Cr3Ag2 square pyramid, edges with two equivalent S(8)TaCr2Ag2 square pyramids, and edges with two equivalent S(6)Ta2CrAg2 trigonal bipyramids. In the seventh S site, S(7) is bonded to one Cr(3), two equivalent Cr(1), and two equivalent Ag(2) atoms to form distorted SCr3Ag2 square pyramids that share corners with two equivalent S(2)Cr2Ag3 square pyramids, corners with two equivalent S(6)Ta2CrAg2 trigonal bipyramids, edges with two equivalent S(7)Cr3Ag2 square pyramids, edges with three equivalent S(2)Cr2Ag3 square pyramids,  an edgeedge with one S(6)Ta2CrAg2 trigonal bipyramid, and edges with two equivalent S(5)Cr3Ag2 trigonal bipyramids. In the eighth S site, S(8) is bonded to one Ta(1), two equivalent Cr(2), and two equivalent Ag(1) atoms to form distorted STaCr2Ag2 square pyramids that share corners with two equivalent S(5)Cr3Ag2 trigonal bipyramids, edges with two equivalent S(8)TaCr2Ag2 square pyramids,  an edgeedge with one S(5)Cr3Ag2 trigonal bipyramid, and edges with two equivalent S(6)Ta2CrAg2 trigonal bipyramids.