NdYbS3 crystallizes in the orthorhombic Cmcm space group. Yb(1) is bonded to two equivalent S(2) and four equivalent S(1) atoms to form a mixture of corner and edge-sharing YbS6 octahedra. The corner-sharing octahedral tilt angles are 68°. Nd(1) is bonded in a 8-coordinate geometry to two equivalent S(2) and six equivalent S(1) atoms. There are two inequivalent S sites. In the first S site, S(1) is bonded to two equivalent Yb(1) and three equivalent Nd(1) atoms to form distorted SYb2Nd3 square pyramids that share corners with nine equivalent S(1)Yb2Nd3 square pyramids, corners with four equivalent S(2)Yb2Nd2 tetrahedra, edges with six equivalent S(1)Yb2Nd3 square pyramids, and edges with three equivalent S(2)Yb2Nd2 tetrahedra. In the second S site, S(2) is bonded to two equivalent Yb(1) and two equivalent Nd(1) atoms to form SYb2Nd2 tetrahedra that share corners with eight equivalent S(1)Yb2Nd3 square pyramids, corners with four equivalent S(2)Yb2Nd2 tetrahedra, and edges with six equivalent S(1)Yb2Nd3 square pyramids.
NdYbS3 crystallizes in the orthorhombic Cmcm space group. Yb(1) is bonded to two equivalent S(2) and four equivalent S(1) atoms to form a mixture of corner and edge-sharing YbS6 octahedra. The corner-sharing octahedral tilt angles are 68°. Both Yb(1)-S(2) bond lengths are 2.68 Å. All Yb(1)-S(1) bond lengths are 2.87 Å. Nd(1) is bonded in a 8-coordinate geometry to two equivalent S(2) and six equivalent S(1) atoms. Both Nd(1)-S(2) bond lengths are 2.77 Å. There are four shorter (2.93 Å) and two longer (3.34 Å) Nd(1)-S(1) bond lengths. There are two inequivalent S sites. In the first S site, S(1) is bonded to two equivalent Yb(1) and three equivalent Nd(1) atoms to form distorted SYb2Nd3 square pyramids that share corners with nine equivalent S(1)Yb2Nd3 square pyramids, corners with four equivalent S(2)Yb2Nd2 tetrahedra, edges with six equivalent S(1)Yb2Nd3 square pyramids, and edges with three equivalent S(2)Yb2Nd2 tetrahedra. In the second S site, S(2) is bonded to two equivalent Yb(1) and two equivalent Nd(1) atoms to form SYb2Nd2 tetrahedra that share corners with eight equivalent S(1)Yb2Nd3 square pyramids, corners with four equivalent S(2)Yb2Nd2 tetrahedra, and edges with six equivalent S(1)Yb2Nd3 square pyramids.