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The electrical and luminescent properties of the GaN epitaxial films grown on AlN‐coated sapphire by reactive molecular beam epitaxy have been studied. The GaN films on AlN epitaxial films have larger Hall mobilities and show more intense cathodoluminescence peaks at a wavelength of 360 nm than those of the GaN films grown directly on sapphire, which suggests that the crystal qualities of GaN films are improved by use of AlN‐coated sapphire as substrates. The lattice matching and small difference of the thermal expansion coefficients between GaN and AlN are considered to result in the improvements.