In this paper, Ni–Cr–Al coatings were deposited using the detonation spraying method. The aim was to investigate how technological parameters influence coating structure formation, phase composition and tribological performances. We observed that the degree to which the barrel is filled with an O2/C2H2 gas mixture strongly influences the chemical composition of manufactured coatings. High degrees of barrel filling led to a decrease in aluminum content in the coating. Filling degrees of 40% and 50% produced sprayed coatings in which only Ni–Cr phases could be found. When the filling degree was reduced up to 25%, Ni–Al phases began to form in the sprayed coatings. Gradient Ni–Cr–Al coatings were produced by gradually reducing the filling degree from 50% to 25%. These coatings are characterized by Ni–Cr near the substrate level with Ni–Cr and Ni–Al phases at higher levels. The results obtained confirm that gradient Ni–Cr–Al coatings exhibit high hardness as well as good wear resistance.