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CaNi2 is Cubic Laves structured and crystallizes in the cubic Fd-3m space group. The structure is three-dimensional. Ca is bonded in a 12-coordinate geometry to twelve equivalent Ni atoms. All Ca–Ni bond lengths are 2.97 Å. Ni is bonded to six equivalent Ca and six equivalent Ni atoms to form a mixture of edge, face, and corner-sharing NiCa6Ni6 cuboctahedra. All Ni–Ni bond lengths are 2.54 Å.
CaNi5 crystallizes in the orthorhombic Imma space group. The structure is three-dimensional. Ca is bonded in a 6-coordinate geometry to eighteen Ni atoms. There are a spread of Ca–Ni bond distances ranging from 2.80–3.22 Å. There are three inequivalent Ni sites. In the first Ni site, Ni is bonded to four equivalent Ca and eight Ni atoms to form a mixture of edge, corner, and face-sharing NiCa4Ni8 cuboctahedra. There are four shorter (2.41 Å) and four longer (2.45 Å) Ni–Ni bond lengths. In the second Ni site, Ni is bonded to four equivalent Ca and eight Ni atoms to form a mixture of edge, corner, and face-sharing NiCa4Ni8 cuboctahedra. There are a spread of Ni–Ni bond distances ranging from 2.41–2.47 Å. In the third Ni site, Ni is bonded in a 3-coordinate geometry to three equivalent Ca and eight Ni atoms. There are one shorter (2.62 Å) and one longer (2.81 Å) Ni–Ni bond lengths.
Ca4Ni is Iron carbide-like structured and crystallizes in the cubic Fd-3m space group. The structure is zero-dimensional and consists of eight Ca4Ni clusters. Ca is bonded in a single-bond geometry to one Ni atom. The Ca–Ni bond length is 2.59 Å. Ni is bonded in a tetrahedral geometry to four equivalent Ca atoms.
CaNi is Tetraauricupride structured and crystallizes in the cubic Pm-3m space group. The structure is three-dimensional. Ca is bonded in a body-centered cubic geometry to eight equivalent Ni atoms. All Ca–Ni bond lengths are 2.97 Å. Ni is bonded in a body-centered cubic geometry to eight equivalent Ca atoms.