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Holographic characteristics of chalcogenide film materials with a typical thickness of 0.5–1.5 µm of a number of Ge-S and As-S compositions have been studied theoretically and experimentally with the aim of using them in augmented reality waveguide devices. The possibility of controlling the spectral and holographic properties of materials by varying their composition is shown. The recording of both volume and surface holographic elements operating in the total internal reflection mode was carried out. The operation of holograms in the “periscope mode” with a diffraction efficiency of about 10% is demonstrated. It is concluded that the recording of high-performance holographic elements on chalcogenide films requires significant values of exposure energy when recording in the near UV range (325–355 nm), which makes holographic recording currently ineffective for creating such elements.