Ca2OsN3 crystallizes in the orthorhombic Cmce space group. There are two inequivalent Ca sites. In the first Ca site, Ca(1) is bonded to two equivalent N(1) and three equivalent N(2) atoms to form distorted CaN5 trigonal bipyramids that share corners with four equivalent Ca(2)N7 pentagonal bipyramids, corners with five equivalent Os(1)N4 tetrahedra, corners with two equivalent Ca(1)N5 trigonal bipyramids, edges with four equivalent Ca(2)N7 pentagonal bipyramids, and edges with three equivalent Ca(1)N5 trigonal bipyramids. In the second Ca site, Ca(2) is bonded to two equivalent N(2), two equivalent N(3), and three equivalent N(1) atoms to form distorted CaN7 pentagonal bipyramids that share corners with four equivalent Ca(2)N7 pentagonal bipyramids,  a cornercorner with one Os(1)N4 tetrahedra, corners with four equivalent Ca(1)N5 trigonal bipyramids, edges with three equivalent Ca(2)N7 pentagonal bipyramids, edges with four equivalent Os(1)N4 tetrahedra, and edges with four equivalent Ca(1)N5 trigonal bipyramids. Os(1) is bonded to one N(1), one N(2), and two equivalent N(3) atoms to form OsN4 tetrahedra that share  a cornercorner with one Ca(2)N7 pentagonal bipyramid, corners with two equivalent Os(1)N4 tetrahedra, corners with five equivalent Ca(1)N5 trigonal bipyramids, and edges with four equivalent Ca(2)N7 pentagonal bipyramids. There are three inequivalent N sites. In the first N site, N(3) is bonded in a 4-coordinate geometry to two equivalent Ca(2) and two equivalent Os(1) atoms. In the second N site, N(1) is bonded to two equivalent Ca(1), three equivalent Ca(2), and one Os(1) atom to form a mixture of distorted corner and edge-sharing NCa5Os octahedra. The corner-sharing octahedral tilt angles range from 12-53°. In the third N site, N(2) is bonded to two equivalent Ca(2), three equivalent Ca(1), and one Os(1) atom to form a mixture of distorted corner and edge-sharing NCa5Os octahedra. The corner-sharing octahedral tilt angles range from 10-53°.
Ca2OsN3 crystallizes in the orthorhombic Cmce space group. There are two inequivalent Ca sites. In the first Ca site, Ca(1) is bonded to two equivalent N(1) and three equivalent N(2) atoms to form distorted CaN5 trigonal bipyramids that share corners with four equivalent Ca(2)N7 pentagonal bipyramids, corners with five equivalent Os(1)N4 tetrahedra, corners with two equivalent Ca(1)N5 trigonal bipyramids, edges with four equivalent Ca(2)N7 pentagonal bipyramids, and edges with three equivalent Ca(1)N5 trigonal bipyramids. There is one shorter (2.32 Å) and one longer (2.58 Å) Ca(1)-N(1) bond length. There is one shorter (2.72 Å) and two longer (2.80 Å) Ca(1)-N(2) bond lengths. In the second Ca site, Ca(2) is bonded to two equivalent N(2), two equivalent N(3), and three equivalent N(1) atoms to form distorted CaN7 pentagonal bipyramids that share corners with four equivalent Ca(2)N7 pentagonal bipyramids,  a cornercorner with one Os(1)N4 tetrahedra, corners with four equivalent Ca(1)N5 trigonal bipyramids, edges with three equivalent Ca(2)N7 pentagonal bipyramids, edges with four equivalent Os(1)N4 tetrahedra, and edges with four equivalent Ca(1)N5 trigonal bipyramids. There is one shorter (2.35 Å) and one longer (2.65 Å) Ca(2)-N(2) bond length. Both Ca(2)-N(3) bond lengths are 2.62 Å. There is one shorter (2.57 Å) and two longer (2.85 Å) Ca(2)-N(1) bond lengths. Os(1) is bonded to one N(1), one N(2), and two equivalent N(3) atoms to form OsN4 tetrahedra that share  a cornercorner with one Ca(2)N7 pentagonal bipyramid, corners with two equivalent Os(1)N4 tetrahedra, corners with five equivalent Ca(1)N5 trigonal bipyramids, and edges with four equivalent Ca(2)N7 pentagonal bipyramids. The Os(1)-N(1) bond length is 1.89 Å. The Os(1)-N(2) bond length is 1.90 Å. Both Os(1)-N(3) bond lengths are 1.88 Å. There are three inequivalent N sites. In the first N site, N(3) is bonded in a 4-coordinate geometry to two equivalent Ca(2) and two equivalent Os(1) atoms. In the second N site, N(1) is bonded to two equivalent Ca(1), three equivalent Ca(2), and one Os(1) atom to form a mixture of distorted corner and edge-sharing NCa5Os octahedra. The corner-sharing octahedral tilt angles range from 12-53°. In the third N site, N(2) is bonded to two equivalent Ca(2), three equivalent Ca(1), and one Os(1) atom to form a mixture of distorted corner and edge-sharing NCa5Os octahedra. The corner-sharing octahedral tilt angles range from 10-53°.