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The growth, structure, and annealing behavior of Al films, formed by in situ vapor deposition on GaN(0001)–(1×1) near 25 °C, have been studied using Auger, electron energy loss, x ray and ultraviolet photoemission spectroscopies and low‐energy electron diffraction. Film growth occurs by a Stranski–Krastanov process with reaction at the immediate interface leading to metallic Ga. Annealing at ≳800 °C leads to release of N, which reacts with Al to form a (1×1)‐ordered layer of AlN, possibly alloyed with a small amount of Ga. The AlN layer has been characterized using the various spectroscopies, and the work function, band bending, and electron affinity of GaN and of the AlN overlayer have been obtained. The Al/GaN Schottky barrier height has been measured and compared with previous results for Ni/GaN.