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Scale-dependent microstructure and electronic transportation of Ni/Al-type nanomultilayers as a function of the bilayers number, the modulated ratio, and the periodicity were investigated. The deposited multilayers have anisotropic nanocrystalline structure and asymmetrical interfaces. This special interfacial feature is the result of asymmetrical diffusion of Ni to Al lattice near the Ni–Al interface. Anomalous resistivity enhancement increases with decreasing both the periodicity and the modulated ratio, but is insensitive to the number of bilayers. Accounting for the effects of grain boundary and interface boundary, the dominative mechanism at distinct length scales can be interpreted with the modified model of those of Fuchs–Sondheimer and Mayadas–Shatzkes. Especially for the thinnest film with smallest modulated ratio, the intermixing effect turns out to be the crucial mechanism in the electronic transportation of metallic nanomultilayers.