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TmNi crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. Tm is bonded in a 7-coordinate geometry to seven equivalent Ni atoms. There are a spread of Tm–Ni bond distances ranging from 2.83–2.89 Å. Ni is bonded in a 9-coordinate geometry to seven equivalent Tm and two equivalent Ni atoms. Both Ni–Ni bond lengths are 2.52 Å.
TmNi5 crystallizes in the hexagonal P6/mmm space group. The structure is three-dimensional. Tm is bonded in a distorted hexagonal planar geometry to eighteen Ni atoms. There are six shorter (2.79 Å) and twelve longer (3.12 Å) Tm–Ni bond lengths. There are two inequivalent Ni sites. In the first Ni site, Ni is bonded in a 12-coordinate geometry to three equivalent Tm and nine Ni atoms. There are six shorter (2.42 Å) and three longer (2.79 Å) Ni–Ni bond lengths. In the second Ni site, Ni is bonded to four equivalent Tm and eight Ni atoms to form a mixture of corner, edge, and face-sharing NiTm4Ni8 cuboctahedra. All Ni–Ni bond lengths are 2.41 Å.
Tm2Ni17 crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. there are two inequivalent Tm sites. In the first Tm site, Tm is bonded in a 12-coordinate geometry to eighteen Ni atoms. There are a spread of Tm–Ni bond distances ranging from 2.89–3.21 Å. In the second Tm site, Tm is bonded in a 2-coordinate geometry to twenty Ni atoms. There are a spread of Tm–Ni bond distances ranging from 2.80–3.10 Å. There are four inequivalent Ni sites. In the first Ni site, Ni is bonded in a 2-coordinate geometry to one Tm and thirteen Ni atoms. There are a spread of Ni–Ni bond distances ranging from 2.38–2.70 Å. In the second Ni site, Ni is bonded to two equivalent Tm and ten Ni atoms to form NiTm2Ni10 cuboctahedra that share corners with fourteen NiTm2Ni10 cuboctahedra, edges with six equivalent NiTm3Ni9 cuboctahedra, and faces with ten NiTm2Ni10 cuboctahedra. There are four shorter (2.37 Å) and four longer (2.39 Å) Ni–Ni bond lengths. In the third Ni site, Ni is bonded in a 12-coordinate geometry to two Tm and ten Ni atoms. There are a spread of Ni–Ni bond distances ranging from 2.35–2.50 Å. In the fourth Ni site, Ni is bonded to three Tm and nine Ni atoms to form a mixture of distorted corner, edge, and face-sharing NiTm3Ni9 cuboctahedra. Both Ni–Ni bond lengths are 2.38 Å.
TmNi2 is Cubic Laves structured and crystallizes in the cubic F-43m space group. The structure is three-dimensional. there are five inequivalent Tm sites. In the first Tm site, Tm is bonded in a 12-coordinate geometry to twelve equivalent Ni atoms. All Tm–Ni bond lengths are 2.95 Å. In the second Tm site, Tm is bonded in a 12-coordinate geometry to twelve equivalent Ni atoms. All Tm–Ni bond lengths are 2.95 Å. In the third Tm site, Tm is bonded in a 12-coordinate geometry to twelve Ni atoms. All Tm–Ni bond lengths are 2.95 Å. In the fourth Tm site, Tm is bonded in a 12-coordinate geometry to twelve Ni atoms. All Tm–Ni bond lengths are 2.95 Å. In the fifth Tm site, Tm is bonded in a 12-coordinate geometry to twelve Ni atoms. There are two shorter (2.94 Å) and ten longer (2.95 Å) Tm–Ni bond lengths. There are four inequivalent Ni sites. In the first Ni site, Ni is bonded to six Tm and six Ni atoms to form a mixture of face, edge, and corner-sharing NiTm6Ni6 cuboctahedra. There are three shorter (2.50 Å) and three longer (2.52 Å) Ni–Ni bond lengths. In the second Ni site, Ni is bonded to six Tm and six Ni atoms to form a mixture of face, edge, and corner-sharing NiTm6Ni6 cuboctahedra. There are three shorter (2.51 Å) and three longer (2.52 Å) Ni–Ni bond lengths. In the third Ni site, Ni is bonded to six Tm and six Ni atoms to form a mixture of face, edge, and corner-sharing NiTm6Ni6 cuboctahedra. There are four shorter (2.51 Å) and one longer (2.52 Å) Ni–Ni bond lengths. In the fourth Ni site, Ni is bonded to six Tm and six Ni atoms to form a mixture of face, edge, and corner-sharing NiTm6Ni6 cuboctahedra. There are one shorter (2.51 Å) and two longer (2.52 Å) Ni–Ni bond lengths.
Tm4Ni is Iron carbide-like structured and crystallizes in the cubic Fd-3m space group. The structure is zero-dimensional and consists of eight Tm4Ni clusters. Tm is bonded in a single-bond geometry to one Ni atom. The Tm–Ni bond length is 2.49 Å. Ni is bonded in a tetrahedral geometry to four equivalent Tm atoms.