V2N2S crystallizes in the trigonal P-3m1 space group. V(1) is bonded to four equivalent N(1) and three equivalent S(1) atoms to form a mixture of distorted corner and edge-sharing VS3N4 trigonal pyramids. N(1) is bonded to four equivalent V(1) atoms to form NV4 trigonal pyramids that share corners with six equivalent S(1)V6 octahedra, corners with six equivalent N(1)V4 trigonal pyramids, edges with three equivalent S(1)V6 octahedra, and edges with three equivalent N(1)V4 trigonal pyramids. The corner-sharing octahedral tilt angles range from 38-46°. S(1) is bonded to six equivalent V(1) atoms to form distorted SV6 octahedra that share corners with twelve equivalent N(1)V4 trigonal pyramids, edges with six equivalent S(1)V6 octahedra, and edges with six equivalent N(1)V4 trigonal pyramids.
V2N2S crystallizes in the trigonal P-3m1 space group. V(1) is bonded to four equivalent N(1) and three equivalent S(1) atoms to form a mixture of distorted corner and edge-sharing VS3N4 trigonal pyramids. There are three shorter (1.94 Å) and one longer (1.97 Å) V(1)-N(1) bond length. All V(1)-S(1) bond lengths are 2.68 Å. N(1) is bonded to four equivalent V(1) atoms to form NV4 trigonal pyramids that share corners with six equivalent S(1)V6 octahedra, corners with six equivalent N(1)V4 trigonal pyramids, edges with three equivalent S(1)V6 octahedra, and edges with three equivalent N(1)V4 trigonal pyramids. The corner-sharing octahedral tilt angles range from 38-46°. S(1) is bonded to six equivalent V(1) atoms to form distorted SV6 octahedra that share corners with twelve equivalent N(1)V4 trigonal pyramids, edges with six equivalent S(1)V6 octahedra, and edges with six equivalent N(1)V4 trigonal pyramids.