An ultrathin nanolaminate (Al2O3/ZrO2/Al2O3) film prepared by atomic layer chemical vapor deposition was investigated for use in metal-oxide-semiconductor field effect transistor (MOSFET) gate dielectric applications. Based on transmission electron microscopy and medium-energy ion scattering spectroscopy (MEIS) analysis, an abrupt interface between stoichiometric top-layer Al2O3 and ZrO2 was found. Interfacial layers such as Zr-Al-O and Al-Si-O were also observed. An electrical equivalent oxide thickness as thin as 10.2 Angstrom with a quantum mechanical correction was obtained. Additional plasma nitridation of nanolaminte in N-2 led to a significant reduction in the interfacial oxidation of nanolaminate which was confirmed by x-ray photoelectron spectroscopy, MEIS, and capacitance-voltage (C-V) analysis. The nanolaminate film represents a promising alternative for gate dielectric applications of future sub-100 nm MOSFET