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NiTi crystallizes in the orthorhombic Cmcm space group. The structure is three-dimensional. Ti is bonded in a 7-coordinate geometry to seven equivalent Ni atoms. There are a spread of Ti–Ni bond distances ranging from 2.54–2.59 Å. Ni is bonded in a 7-coordinate geometry to seven equivalent Ti atoms.
Ti3Ni is beta Cu3Ti-like structured and crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Ti is bonded to eight equivalent Ti and four equivalent Ni atoms to form distorted TiTi8Ni4 cuboctahedra that share corners with four equivalent NiTi12 cuboctahedra, corners with fourteen equivalent TiTi8Ni4 cuboctahedra, edges with six equivalent NiTi12 cuboctahedra, edges with twelve equivalent TiTi8Ni4 cuboctahedra, faces with four equivalent NiTi12 cuboctahedra, and faces with sixteen equivalent TiTi8Ni4 cuboctahedra. There are two shorter (2.62 Å) and six longer (2.83 Å) Ti–Ti bond lengths. There are two shorter (2.72 Å) and two longer (2.76 Å) Ti–Ni bond lengths. Ni is bonded to twelve equivalent Ti atoms to form NiTi12 cuboctahedra that share corners with six equivalent NiTi12 cuboctahedra, corners with twelve equivalent TiTi8Ni4 cuboctahedra, edges with eighteen equivalent TiTi8Ni4 cuboctahedra, faces with eight equivalent NiTi12 cuboctahedra, and faces with twelve equivalent TiTi8Ni4 cuboctahedra.