Epitaxially grown, chemically homogeneous yttria-stabilized zirconia thin films ("YSZ", 8 mol% Y2O3) are prepared by direct-current sputtering onto a single-crystalline NaCl(0 0 1) template at substrate temperatures >= 493 K, resulting in unsupported YSZ films after floating off NaCl in water. A combined methodological approach by dedicated (surface science) analytical characterization tools (transmission electron microscopy and diffraction, atomic force microscopy, angle-resolved X-ray photoelectron spectroscopy) reveals that the film grows mainly in a [0 0 1] zone axis and no Y-enrichment in surface or bulk regions takes place. In fact, the Y-content of the sputter target is preserved in the thin films. Analysis of the plasmon region in EEL spectra indicates a defective nature of the as-deposited films, which can be suppressed by post-deposition oxidation at 1073 K. This, however, induces considerable sintering, as deduced from surface morphology measurements by AFM. In due course, the so-prepared unsupported YSZ films might act as well-defined model systems also for technological applications. (C) 2015 Elsevier B.V. All rights reserved.