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NiTe2 is Calaverite structured and crystallizes in the trigonal P-3m1 space group. The structure is two-dimensional and consists of one NiTe2 sheet oriented in the (0, 0, 1) direction. Ni4+ is bonded to six equivalent Te2- atoms to form edge-sharing NiTe6 octahedra. All Ni–Te bond lengths are 2.60 Å. Te2- is bonded in a 3-coordinate geometry to three equivalent Ni4+ atoms.
NiTe2 is pyrite-like structured and crystallizes in the cubic Pa-3 space group. The structure is three-dimensional. Ni4+ is bonded to six equivalent Te2- atoms to form corner-sharing NiTe6 octahedra. The corner-sharing octahedral tilt angles are 61°. All Ni–Te bond lengths are 2.63 Å. Te2- is bonded in a distorted trigonal planar geometry to three equivalent Ni4+ atoms.