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AgI–Al2O3 nanocomposites are investigated by high-resolution electron microscopy and luminescence spectroscopy. The results show that both crystalline and amorphous phases coexist in AgI–Al2O3 composites. At sufficiently high alumina content, almost all AgI occurs as amorphous spherical nanoparticles distributed uniformly on alumina surfaces. The amorphous phase exhibits unusual luminescence spectra with a single, very broad nonstructured band. The amorphous phase is stabilized on AgI–alumina interfaces with the relative concentration progressively increasing with the Al2O3 fraction. The thickness of the interface amorphous layer adjacent to Al2O3 particles estimated by means of a simple brick-wall model is about 3 nm.