The performance of atmospheric plasma sprayed FeAl coatings has been remarkably limited because of oxidation and phase transformation during the high-temperature process of preparation. In the present work, FeAl intermetallic coatings were prepared by atmospheric plasma spraying combined with dry-ice blasting. The microstructure, oxidation, porosity, and surface roughness of FeAl intermetallic coatings were investigated. The results show that a denser FeAl coating with a lower content of oxide and lower degree of phase transformation can be achieved because of the cryogenic, the cleaning, and the mechanical effects of dry-ice blasting. The surface roughness value decreased, and the adhesive strength of FeAl coating increased after the application of dry-ice blasting during the atmospheric plasma spraying process. Moreover, the microhardness of the FeAl coating increased by 72%, due to the lower porosity and higher dislocation density.