The use of atomic layer deposition (ALD) to form a nanolaminate layered dielectric layer of cerium oxide and aluminum oxide acting as a single dielectric layer with a ratio of approximately two to one between the cerium oxide and the aluminum oxide, and a method of fabricating such a dielectric layer is described. The described arrangement produces a reliable structure with a high dielectric constant (high-k) for use in a variety of electronic devices. The dielectric structure is formed by depositing cerium oxide by atomic layer deposition onto a substrate surface using precursor chemicals, followed by depositing aluminum oxide onto the substrate using precursor chemicals, and repeating to form the thin laminate structure. Such a dielectric layer of cerium oxide and aluminum oxide may be used as the gate insulator of a MOSFET, as a capacitor dielectric in a DRAM, as a tunnel gate insulator in flash memory, or as a dielectric in an NROM device, because the high dielectric constant (high-k) of the film provides the functionality of a much thinner silicon dioxide film.