Ca4N4Te crystallizes in the triclinic P-1 space group. There are four inequivalent Ca sites. In the first Ca site, Ca(1) is bonded in a 5-coordinate geometry to one N(1), one N(3), one N(4), and two equivalent N(2) atoms. In the second Ca site, Ca(2) is bonded in a 4-coordinate geometry to two equivalent N(2) and two equivalent N(3) atoms. In the third Ca site, Ca(3) is bonded to one N(3), two equivalent N(1), and two equivalent N(4) atoms to form distorted edge-sharing CaN5 trigonal bipyramids. In the fourth Ca site, Ca(4) is bonded in a distorted see-saw-like geometry to two equivalent N(1) and two equivalent N(4) atoms. There are four inequivalent N sites. In the first N site, N(1) is bonded to one Ca(1), two equivalent Ca(3), two equivalent Ca(4), and one Te(1) atom to form distorted NCa5Te octahedra that share corners with three equivalent N(4)Ca5 square pyramids,  a cornercorner with one N(2)Ca4Te trigonal bipyramid, corners with two equivalent N(3)Ca4Te trigonal bipyramids, edges with two equivalent N(1)Ca5Te octahedra, edges with three equivalent N(4)Ca5 square pyramids,  an edgeedge with one N(2)Ca4Te trigonal bipyramid, and  an edgeedge with one N(3)Ca4Te trigonal bipyramid. In the second N site, N(2) is bonded to two equivalent Ca(1), two equivalent Ca(2), and one Te(1) atom to form distorted NCa4Te trigonal bipyramids that share  a cornercorner with one N(1)Ca5Te octahedra, corners with two equivalent N(4)Ca5 square pyramids, corners with five equivalent N(3)Ca4Te trigonal bipyramids,  an edgeedge with one N(1)Ca5Te octahedra,  an edgeedge with one N(3)Ca4Te trigonal bipyramid, and edges with two equivalent N(2)Ca4Te trigonal bipyramids. The corner-sharing octahedral tilt angles are 53°. In the third N site, N(3) is bonded to one Ca(1), one Ca(3), two equivalent Ca(2), and one Te(1) atom to form distorted NCa4Te trigonal bipyramids that share corners with two equivalent N(1)Ca5Te octahedra,  a cornercorner with one N(4)Ca5 square pyramid, corners with five equivalent N(2)Ca4Te trigonal bipyramids,  an edgeedge with one N(1)Ca5Te octahedra,  an edgeedge with one N(4)Ca5 square pyramid,  an edgeedge with one N(2)Ca4Te trigonal bipyramid, and  an edgeedge with one N(3)Ca4Te trigonal bipyramid. The corner-sharing octahedral tilt angles range from 28-69°. In the fourth N site, N(4) is bonded to one Ca(1), two equivalent Ca(3), and two equivalent Ca(4) atoms to form NCa5 square pyramids that share corners with three equivalent N(1)Ca5Te octahedra,  a cornercorner with one N(3)Ca4Te trigonal bipyramid, corners with two equivalent N(2)Ca4Te trigonal bipyramids, edges with three equivalent N(1)Ca5Te octahedra, edges with two equivalent N(4)Ca5 square pyramids, and  an edgeedge with one N(3)Ca4Te trigonal bipyramid. The corner-sharing octahedral tilt angles range from 14-81°. Te(1) is bonded in a distorted trigonal non-coplanar geometry to one N(1), one N(2), and one N(3) atom.
Ca4N4Te crystallizes in the triclinic P-1 space group. There are four inequivalent Ca sites. In the first Ca site, Ca(1) is bonded in a 5-coordinate geometry to one N(1), one N(3), one N(4), and two equivalent N(2) atoms. The Ca(1)-N(1) bond length is 2.74 Å. The Ca(1)-N(3) bond length is 2.52 Å. The Ca(1)-N(4) bond length is 2.36 Å. There is one shorter (2.60 Å) and one longer (2.69 Å) Ca(1)-N(2) bond length. In the second Ca site, Ca(2) is bonded in a 4-coordinate geometry to two equivalent N(2) and two equivalent N(3) atoms. There is one shorter (2.31 Å) and one longer (2.59 Å) Ca(2)-N(2) bond length. There is one shorter (2.45 Å) and one longer (2.50 Å) Ca(2)-N(3) bond length. In the third Ca site, Ca(3) is bonded to one N(3), two equivalent N(1), and two equivalent N(4) atoms to form distorted edge-sharing CaN5 trigonal bipyramids. The Ca(3)-N(3) bond length is 2.48 Å. There is one shorter (2.43 Å) and one longer (2.69 Å) Ca(3)-N(1) bond length. There is one shorter (2.29 Å) and one longer (2.50 Å) Ca(3)-N(4) bond length. In the fourth Ca site, Ca(4) is bonded in a distorted see-saw-like geometry to two equivalent N(1) and two equivalent N(4) atoms. There is one shorter (2.54 Å) and one longer (2.55 Å) Ca(4)-N(1) bond length. There is one shorter (2.31 Å) and one longer (2.37 Å) Ca(4)-N(4) bond length. There are four inequivalent N sites. In the first N site, N(1) is bonded to one Ca(1), two equivalent Ca(3), two equivalent Ca(4), and one Te(1) atom to form distorted NCa5Te octahedra that share corners with three equivalent N(4)Ca5 square pyramids,  a cornercorner with one N(2)Ca4Te trigonal bipyramid, corners with two equivalent N(3)Ca4Te trigonal bipyramids, edges with two equivalent N(1)Ca5Te octahedra, edges with three equivalent N(4)Ca5 square pyramids,  an edgeedge with one N(2)Ca4Te trigonal bipyramid, and  an edgeedge with one N(3)Ca4Te trigonal bipyramid. The N(1)-Te(1) bond length is 2.00 Å. In the second N site, N(2) is bonded to two equivalent Ca(1), two equivalent Ca(2), and one Te(1) atom to form distorted NCa4Te trigonal bipyramids that share  a cornercorner with one N(1)Ca5Te octahedra, corners with two equivalent N(4)Ca5 square pyramids, corners with five equivalent N(3)Ca4Te trigonal bipyramids,  an edgeedge with one N(1)Ca5Te octahedra,  an edgeedge with one N(3)Ca4Te trigonal bipyramid, and edges with two equivalent N(2)Ca4Te trigonal bipyramids. The corner-sharing octahedral tilt angles are 53°. The N(2)-Te(1) bond length is 2.04 Å. In the third N site, N(3) is bonded to one Ca(1), one Ca(3), two equivalent Ca(2), and one Te(1) atom to form distorted NCa4Te trigonal bipyramids that share corners with two equivalent N(1)Ca5Te octahedra,  a cornercorner with one N(4)Ca5 square pyramid, corners with five equivalent N(2)Ca4Te trigonal bipyramids,  an edgeedge with one N(1)Ca5Te octahedra,  an edgeedge with one N(4)Ca5 square pyramid,  an edgeedge with one N(2)Ca4Te trigonal bipyramid, and  an edgeedge with one N(3)Ca4Te trigonal bipyramid. The corner-sharing octahedral tilt angles range from 28-69°. The N(3)-Te(1) bond length is 2.04 Å. In the fourth N site, N(4) is bonded to one Ca(1), two equivalent Ca(3), and two equivalent Ca(4) atoms to form NCa5 square pyramids that share corners with three equivalent N(1)Ca5Te octahedra,  a cornercorner with one N(3)Ca4Te trigonal bipyramid, corners with two equivalent N(2)Ca4Te trigonal bipyramids, edges with three equivalent N(1)Ca5Te octahedra, edges with two equivalent N(4)Ca5 square pyramids, and  an edgeedge with one N(3)Ca4Te trigonal bipyramid. The corner-sharing octahedral tilt angles range from 14-81°. Te(1) is bonded in a distorted trigonal non-coplanar geometry to one N(1), one N(2), and one N(3) atom.