Amorphous, 200 nm thin multilayer structures (including films composed of the pure constituents) and homogeneously mixed films, respectively, were prepared by alternating deposition and co-deposition of alumina and zirconia. Subsequent heating of the films showed crystallization temperatures between 850 and 950°C. At 1000°C, the selective crystallization of metastable cubic zirconia was observed. The elastoplastic properties of the amorphous films were examined using ultra-low load indentation tests. The hardness and the Young's modulus of multilayer structures varied linearly with the overall alumina-zirconia composition. Homogeneously mixed films, by contrast, deviated from such a linear relationship. They exhibited a hardness higher than even alumina films and simultaneously a Young's modulus lower than even zirconia films over a wide concentration range. Different proportionalities between hardness and Young's modulus were observed for the multilayer and the homogeneous films. These results indicate that the molecular mixing of the cpnstituents led to an increase of both the yield strength and the maximum elastic tensile strain.