Epitaxial VNi2 layers are deposited onto MgO(001) and their resistivity ρ measured as a function of layer thickness d = 10.5–138 nm to quantify the resistivity size effect. The layers exhibit resistivity minima at both stoichiometric V:Ni = 1:2 composition and 700 °C growth temperature, which is attributed to electron scattering at V–Ni antisite defects and is described using the ordering parameter within the framework by Rossiter. A cube-on-cube epitaxy of the fcc parent structure on MgO(001) leads to two possible layer orientations for orthorhombic VNi2(010) and VNi2(103), resulting in considerable atomic disorder at domain boundaries, consistent with relatively small x-ray coherence lengths of 8 and 14 nm in-plane and along the growth direction of a 33.5 nm thick layer. In situ ρ vs d measurements yield a bulk resistivity of ρo = 46 ± 2 μ Ω cm and a benchmark quantity of ρoλ = (138 ± 5) × 10−16 Ω m2, where λ is the bulk electron mean free path. Air exposure causes a minor resistivity increase due to 2 ± 1 nm thick surface oxide that perturbs the surface potential. Resistivities at 77 K are Δρ = 16 ± 3 μ Ω cm below those at room temperature. This Δρ is thickness independent and is close to the previously predicted 13.9 μ Ω cm bulk resistivity for VNi2 along [100]. However, the measured bulk resistivity is well above this prediction, which is attributed to electron scattering at domain boundaries/atomic disorder. Consequently, the theoretically predicted superior directional conduction cannot be experimentally confirmed in this study. The overall results indicate that VNi2 is only a promising compound for narrow interconnects if a synthesis scheme can be developed that results in a strong atomic order, a negligible domain boundary density, and a [100] crystalline orientation along the transport direction.

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