An analytical high-resolution electron microscopy study of Y2O3 and ZrO2 thin films, being relevant oxide model systems for a range of industrial applications, is reported. Both films were deposited on vacuum-cleaved NaCl(001) single crystal planes at varying substrate temperatures. A transition from an amorphous to a well-defined and -ordered structure, exhibiting almost single-crystalline ordering of either body-centered cubic Y2O3 or tetragonal ZrO2, both with uniform electronic structure, has been observed upon raising the substrate temperature from 300 to 573 K. Pronounced crystallographic relationships between the face-centered cubic NaCl structure and the structures of the deposited oxides have been held responsible for the observed epitaxial growth. In summary, the chosen preparation pathway represents an easy and reproducible method to yield well-defined oxide structures at surprisingly low substrate temperatures being at the same time promising model candidates for materials-related (e.g. solid-oxide fuel cell) research. With respect to solid-oxide fuel cell technology, monitoring carbon deposition and reactivity following high-temperature treatments in hydrocarbon-containing gas feeds or the use as templates or supports for model systems of realistic anode materials on metallic or bimetallic basis are envisioned application areas. (C) 2012 Elsevier B.V. All rights reserved.