Nanostructured aluminum-nitride films are formed by reactive ion-plasma sputtering onto GaAs substrates with different orientations. The properties of the films are studied via structural analysis, atomic force microscopy, and infrared and visible–ultraviolet spectroscopy. The aluminum-nitride films can have a refractive index in the range of 1.6–4.0 at a wavelength of ~250 nm and an optical band gap of ~5 eV. It is shown that the morphology, surface composition, and optical characteristics of AlN/GaAs heterophase systems can be controlled using misoriented GaAs substrates.