NdNi4Al crystallizes in the hexagonal P-6m2 space group. Nd(1) is bonded in a 18-coordinate geometry to three equivalent Ni(1), twelve equivalent Ni(2), and three equivalent Al(1) atoms. There are two inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to three equivalent Nd(1), six equivalent Ni(2), and three equivalent Al(1) atoms to form NiNd3Al3Ni6 cuboctahedra that share corners with nine equivalent Al(1)Nd3Ni9 cuboctahedra, corners with twelve equivalent Ni(2)Nd4Al2Ni6 cuboctahedra, edges with six equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, faces with two equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, faces with three equivalent Al(1)Nd3Ni9 cuboctahedra, and faces with eighteen equivalent Ni(2)Nd4Al2Ni6 cuboctahedra. In the second Ni site, Ni(2) is bonded to four equivalent Nd(1), two equivalent Ni(1), four equivalent Ni(2), and two equivalent Al(1) atoms to form distorted NiNd4Al2Ni6 cuboctahedra that share corners with four equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, corners with four equivalent Al(1)Nd3Ni9 cuboctahedra, corners with sixteen equivalent Ni(2)Nd4Al2Ni6 cuboctahedra, edges with ten equivalent Ni(2)Nd4Al2Ni6 cuboctahedra, faces with six equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, faces with six equivalent Al(1)Nd3Ni9 cuboctahedra, and faces with ten equivalent Ni(2)Nd4Al2Ni6 cuboctahedra. Al(1) is bonded to three equivalent Nd(1), three equivalent Ni(1), and six equivalent Ni(2) atoms to form distorted AlNd3Ni9 cuboctahedra that share corners with nine equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, corners with twelve equivalent Ni(2)Nd4Al2Ni6 cuboctahedra, edges with six equivalent Al(1)Nd3Ni9 cuboctahedra, faces with two equivalent Al(1)Nd3Ni9 cuboctahedra, faces with three equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, and faces with eighteen equivalent Ni(2)Nd4Al2Ni6 cuboctahedra.
NdNi4Al crystallizes in the hexagonal P-6m2 space group. Nd(1) is bonded in a 18-coordinate geometry to three equivalent Ni(1), twelve equivalent Ni(2), and three equivalent Al(1) atoms. All Nd(1)-Ni(1) bond lengths are 2.97 Å. All Nd(1)-Ni(2) bond lengths are 3.22 Å. All Nd(1)-Al(1) bond lengths are 2.97 Å. There are two inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to three equivalent Nd(1), six equivalent Ni(2), and three equivalent Al(1) atoms to form NiNd3Al3Ni6 cuboctahedra that share corners with nine equivalent Al(1)Nd3Ni9 cuboctahedra, corners with twelve equivalent Ni(2)Nd4Al2Ni6 cuboctahedra, edges with six equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, faces with two equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, faces with three equivalent Al(1)Nd3Ni9 cuboctahedra, and faces with eighteen equivalent Ni(2)Nd4Al2Ni6 cuboctahedra. All Ni(1)-Ni(2) bond lengths are 2.43 Å. All Ni(1)-Al(1) bond lengths are 2.97 Å. In the second Ni site, Ni(2) is bonded to four equivalent Nd(1), two equivalent Ni(1), four equivalent Ni(2), and two equivalent Al(1) atoms to form distorted NiNd4Al2Ni6 cuboctahedra that share corners with four equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, corners with four equivalent Al(1)Nd3Ni9 cuboctahedra, corners with sixteen equivalent Ni(2)Nd4Al2Ni6 cuboctahedra, edges with ten equivalent Ni(2)Nd4Al2Ni6 cuboctahedra, faces with six equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, faces with six equivalent Al(1)Nd3Ni9 cuboctahedra, and faces with ten equivalent Ni(2)Nd4Al2Ni6 cuboctahedra. There are two shorter (2.53 Å) and two longer (2.61 Å) Ni(2)-Ni(2) bond lengths. Both Ni(2)-Al(1) bond lengths are 2.45 Å. Al(1) is bonded to three equivalent Nd(1), three equivalent Ni(1), and six equivalent Ni(2) atoms to form distorted AlNd3Ni9 cuboctahedra that share corners with nine equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, corners with twelve equivalent Ni(2)Nd4Al2Ni6 cuboctahedra, edges with six equivalent Al(1)Nd3Ni9 cuboctahedra, faces with two equivalent Al(1)Nd3Ni9 cuboctahedra, faces with three equivalent Ni(1)Nd3Al3Ni6 cuboctahedra, and faces with eighteen equivalent Ni(2)Nd4Al2Ni6 cuboctahedra.