NdLaNi2 crystallizes in the monoclinic P2/m space group. There are three inequivalent Nd sites. In the first Nd site, Nd(1) is bonded in a square co-planar geometry to four equivalent Ni(2) and four equivalent Ni(3) atoms. In the second Nd site, Nd(2) is bonded in a square co-planar geometry to four equivalent Ni(1) and four equivalent Ni(3) atoms. In the third Nd site, Nd(3) is bonded in a square co-planar geometry to four equivalent Ni(2) and four equivalent Ni(3) atoms. There are two inequivalent La sites. In the first La site, La(1) is bonded in a square co-planar geometry to two equivalent Ni(1), two equivalent Ni(2), and four equivalent Ni(3) atoms. In the second La site, La(2) is bonded in a square co-planar geometry to four equivalent Ni(1) and four equivalent Ni(3) atoms. There are three inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to two equivalent Nd(2), two equivalent La(1), and two equivalent La(2) atoms to form distorted NiLa4Nd2 pentagonal pyramids that share corners with two equivalent Ni(2)La2Nd4 pentagonal pyramids, corners with four equivalent Ni(1)La4Nd2 pentagonal pyramids, edges with six equivalent Ni(3)La6Nd6 cuboctahedra,  an edgeedge with one Ni(2)La2Nd4 pentagonal pyramid, edges with two equivalent Ni(1)La4Nd2 pentagonal pyramids, faces with three equivalent Ni(3)La6Nd6 cuboctahedra, and faces with two equivalent Ni(1)La4Nd2 pentagonal pyramids. In the second Ni site, Ni(2) is bonded to two equivalent Nd(1), two equivalent Nd(3), and two equivalent La(1) atoms to form distorted NiLa2Nd4 pentagonal pyramids that share corners with two equivalent Ni(1)La4Nd2 pentagonal pyramids, corners with four equivalent Ni(2)La2Nd4 pentagonal pyramids, edges with six equivalent Ni(3)La6Nd6 cuboctahedra,  an edgeedge with one Ni(1)La4Nd2 pentagonal pyramid, edges with two equivalent Ni(2)La2Nd4 pentagonal pyramids, faces with three equivalent Ni(3)La6Nd6 cuboctahedra, and faces with two equivalent Ni(2)La2Nd4 pentagonal pyramids. In the third Ni site, Ni(3) is bonded to two equivalent Nd(1), two equivalent Nd(2), two equivalent Nd(3), two equivalent La(2), and four equivalent La(1) atoms to form NiLa6Nd6 cuboctahedra that share corners with twelve equivalent Ni(3)La6Nd6 cuboctahedra, edges with six equivalent Ni(3)La6Nd6 cuboctahedra, edges with six equivalent Ni(2)La2Nd4 pentagonal pyramids, edges with six equivalent Ni(1)La4Nd2 pentagonal pyramids, faces with two equivalent Ni(3)La6Nd6 cuboctahedra, faces with three equivalent Ni(2)La2Nd4 pentagonal pyramids, and faces with three equivalent Ni(1)La4Nd2 pentagonal pyramids.
NdLaNi2 crystallizes in the monoclinic P2/m space group. There are three inequivalent Nd sites. In the first Nd site, Nd(1) is bonded in a square co-planar geometry to four equivalent Ni(2) and four equivalent Ni(3) atoms. All Nd(1)-Ni(2) bond lengths are 2.77 Å. All Nd(1)-Ni(3) bond lengths are 3.97 Å. In the second Nd site, Nd(2) is bonded in a square co-planar geometry to four equivalent Ni(1) and four equivalent Ni(3) atoms. All Nd(2)-Ni(1) bond lengths are 2.77 Å. All Nd(2)-Ni(3) bond lengths are 3.99 Å. In the third Nd site, Nd(3) is bonded in a square co-planar geometry to four equivalent Ni(2) and four equivalent Ni(3) atoms. All Nd(3)-Ni(2) bond lengths are 2.77 Å. All Nd(3)-Ni(3) bond lengths are 3.99 Å. There are two inequivalent La sites. In the first La site, La(1) is bonded in a square co-planar geometry to two equivalent Ni(1), two equivalent Ni(2), and four equivalent Ni(3) atoms. Both La(1)-Ni(1) bond lengths are 2.77 Å. Both La(1)-Ni(2) bond lengths are 2.75 Å. There are two shorter (3.97 Å) and two longer (4.00 Å) La(1)-Ni(3) bond lengths. In the second La site, La(2) is bonded in a square co-planar geometry to four equivalent Ni(1) and four equivalent Ni(3) atoms. All La(2)-Ni(1) bond lengths are 2.76 Å. All La(2)-Ni(3) bond lengths are 3.98 Å. There are three inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to two equivalent Nd(2), two equivalent La(1), and two equivalent La(2) atoms to form distorted NiLa4Nd2 pentagonal pyramids that share corners with two equivalent Ni(2)La2Nd4 pentagonal pyramids, corners with four equivalent Ni(1)La4Nd2 pentagonal pyramids, edges with six equivalent Ni(3)La6Nd6 cuboctahedra,  an edgeedge with one Ni(2)La2Nd4 pentagonal pyramid, edges with two equivalent Ni(1)La4Nd2 pentagonal pyramids, faces with three equivalent Ni(3)La6Nd6 cuboctahedra, and faces with two equivalent Ni(1)La4Nd2 pentagonal pyramids. In the second Ni site, Ni(2) is bonded to two equivalent Nd(1), two equivalent Nd(3), and two equivalent La(1) atoms to form distorted NiLa2Nd4 pentagonal pyramids that share corners with two equivalent Ni(1)La4Nd2 pentagonal pyramids, corners with four equivalent Ni(2)La2Nd4 pentagonal pyramids, edges with six equivalent Ni(3)La6Nd6 cuboctahedra,  an edgeedge with one Ni(1)La4Nd2 pentagonal pyramid, edges with two equivalent Ni(2)La2Nd4 pentagonal pyramids, faces with three equivalent Ni(3)La6Nd6 cuboctahedra, and faces with two equivalent Ni(2)La2Nd4 pentagonal pyramids. In the third Ni site, Ni(3) is bonded to two equivalent Nd(1), two equivalent Nd(2), two equivalent Nd(3), two equivalent La(2), and four equivalent La(1) atoms to form NiLa6Nd6 cuboctahedra that share corners with twelve equivalent Ni(3)La6Nd6 cuboctahedra, edges with six equivalent Ni(3)La6Nd6 cuboctahedra, edges with six equivalent Ni(2)La2Nd4 pentagonal pyramids, edges with six equivalent Ni(1)La4Nd2 pentagonal pyramids, faces with two equivalent Ni(3)La6Nd6 cuboctahedra, faces with three equivalent Ni(2)La2Nd4 pentagonal pyramids, and faces with three equivalent Ni(1)La4Nd2 pentagonal pyramids.