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The paper describes the development of methods for hardening of pieces of aluminum alloys by ion-induced deposition of Cr–N films. We investigated the nitrogen distribution in the films and in the aluminum substrate. The method of secondary ion mass-spectrometry (SIMS) and a nuclear reaction method (NRM) were used in the study described. A computer model was developed that allowed us to describe the nitrogen distribution under the high temperatures in the growing film and in the interface substrate layers. The experimental results obtained agree well with the calculated data.