Al-Cu-Fe quasicrystalline coatings, due to their high hardness and low friction coefficients, are potential candidates for improving the wear resistance of ductile materials. However, technological applications may be limited on account of their brittle nature. This study examines the effects of starting powder composition and thermal spray process parameters on the phase assemblage, microstructure, and tribological response of Al-Cu-Fe thermally sprayed coatings. It was found that the coatings fail by a delamination mechanism in unlubricated unidirectional sliding wear. Furthermore, the coatings produced by the high velocity oxy-fuel technique showed a very low coefficient of friction and wear rate.