Lattice mismatch stresses, which severely restrict heteroepitaxial growth, are greatly minimized when thin alumina films are grown by means of van der Waals forces on inert mica substrates. A 10-nanometer-thick epitaxial film exhibits crystallographic sixfold symmetry, a lattice constant close to that of the basal plane [0001] of α-alumina (sapphire), and an aluminum:oxygen atomic ratio of 1:1.51 ± 0.02 (measured by x-ray photoelectron spectroscopy), again the same as for bulk sapphire. The film is free of steps and grain boundaries over large areas and appears to be an ideal model system for studying adhesion, tribology, and other surface phenomena at atomic scales.