An ultrathin aluminum oxide and lanthanide layers, particularly formed by an atomic layer deposition (ALD) type process, serve as interface layers between two or more materials. The interface layers can prevent oxidation of a substrate and can prevent diffusion of molecules between the materials. In the illustrated embodiments, a high-k dielectric material is sandwiched between two layers of aluminum oxide or lanthanide oxide in the formation of a transistor gate dielectric or a memory cell dielectric. Aluminum oxides can serve as a nucleation layer with less than a full monolayer of aluminum oxide. One monolayer or greater can also serve as a diffusion barrier, protecting the substrate from oxidation and the high-k dielectric from impurity diffusion. Nanolaminates can be formed with multiple alternating interface layers and high-k layers, where intermediate interface layers can break up the crystal structure of the high-k materials and lower leakage levels.