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MgTiNi2 crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two MgTiNi2 ribbons oriented in the (1, 0, 0) direction. Mg is bonded in a linear geometry to two equivalent Ni atoms. Both Mg–Ni bond lengths are 2.63 Å. Ti is bonded in a linear geometry to two equivalent Ni atoms. Both Ti–Ni bond lengths are 2.07 Å. Ni is bonded in a linear geometry to one Mg and one Ti atom.
Mg3TiNi2 crystallizes in the cubic Fd-3m space group. The structure is three-dimensional. Mg is bonded in a 2-coordinate geometry to eight equivalent Mg, two equivalent Ti, and four equivalent Ni atoms. There are four shorter (3.06 Å) and four longer (3.17 Å) Mg–Mg bond lengths. Both Mg–Ti bond lengths are 2.95 Å. There are two shorter (2.80 Å) and two longer (2.95 Å) Mg–Ni bond lengths. Ti is bonded to six equivalent Mg and six equivalent Ni atoms to form distorted face-sharing TiMg6Ni6 cuboctahedra. All Ti–Ni bond lengths are 2.50 Å. Ni is bonded in a 12-coordinate geometry to six equivalent Mg, three equivalent Ti, and three equivalent Ni atoms. All Ni–Ni bond lengths are 2.65 Å.