TbNi4Fe crystallizes in the hexagonal P-6m2 space group. Tb(1) is bonded in a 18-coordinate geometry to three equivalent Fe(1), three equivalent Ni(1), and twelve equivalent Ni(2) atoms. Fe(1) is bonded to three equivalent Tb(1), three equivalent Ni(1), and six equivalent Ni(2) atoms to form distorted FeTb3Ni9 cuboctahedra that share corners with nine equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, corners with twelve equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra, edges with six equivalent Fe(1)Tb3Ni9 cuboctahedra, faces with two equivalent Fe(1)Tb3Ni9 cuboctahedra, faces with three equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, and faces with eighteen equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra. There are two inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to three equivalent Tb(1), three equivalent Fe(1), and six equivalent Ni(2) atoms to form distorted NiTb3Fe3Ni6 cuboctahedra that share corners with nine equivalent Fe(1)Tb3Ni9 cuboctahedra, corners with twelve equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra, edges with six equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, faces with two equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, faces with three equivalent Fe(1)Tb3Ni9 cuboctahedra, and faces with eighteen equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra. In the second Ni site, Ni(2) is bonded to four equivalent Tb(1), two equivalent Fe(1), two equivalent Ni(1), and four equivalent Ni(2) atoms to form NiTb4Fe2Ni6 cuboctahedra that share corners with four equivalent Fe(1)Tb3Ni9 cuboctahedra, corners with four equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, corners with sixteen equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra, edges with ten equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra, faces with six equivalent Fe(1)Tb3Ni9 cuboctahedra, faces with six equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, and faces with ten equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra.
TbNi4Fe crystallizes in the hexagonal P-6m2 space group. Tb(1) is bonded in a 18-coordinate geometry to three equivalent Fe(1), three equivalent Ni(1), and twelve equivalent Ni(2) atoms. All Tb(1)-Fe(1) bond lengths are 2.85 Å. All Tb(1)-Ni(1) bond lengths are 2.85 Å. All Tb(1)-Ni(2) bond lengths are 3.16 Å. Fe(1) is bonded to three equivalent Tb(1), three equivalent Ni(1), and six equivalent Ni(2) atoms to form distorted FeTb3Ni9 cuboctahedra that share corners with nine equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, corners with twelve equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra, edges with six equivalent Fe(1)Tb3Ni9 cuboctahedra, faces with two equivalent Fe(1)Tb3Ni9 cuboctahedra, faces with three equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, and faces with eighteen equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra. All Fe(1)-Ni(1) bond lengths are 2.85 Å. All Fe(1)-Ni(2) bond lengths are 2.43 Å. There are two inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to three equivalent Tb(1), three equivalent Fe(1), and six equivalent Ni(2) atoms to form distorted NiTb3Fe3Ni6 cuboctahedra that share corners with nine equivalent Fe(1)Tb3Ni9 cuboctahedra, corners with twelve equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra, edges with six equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, faces with two equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, faces with three equivalent Fe(1)Tb3Ni9 cuboctahedra, and faces with eighteen equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra. All Ni(1)-Ni(2) bond lengths are 2.42 Å. In the second Ni site, Ni(2) is bonded to four equivalent Tb(1), two equivalent Fe(1), two equivalent Ni(1), and four equivalent Ni(2) atoms to form NiTb4Fe2Ni6 cuboctahedra that share corners with four equivalent Fe(1)Tb3Ni9 cuboctahedra, corners with four equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, corners with sixteen equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra, edges with ten equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra, faces with six equivalent Fe(1)Tb3Ni9 cuboctahedra, faces with six equivalent Ni(1)Tb3Fe3Ni6 cuboctahedra, and faces with ten equivalent Ni(2)Tb4Fe2Ni6 cuboctahedra. There are two shorter (2.47 Å) and two longer (2.48 Å) Ni(2)-Ni(2) bond lengths.