Well-adhered alumina washcoats on FeCrAl metallic supports were prepared using boehmite sols and alumina slurries. The microstructure and the surface performance of the washcoat/support were investigated by SEM, XRD, and ultrasonic vibration. The effects of the main preparative parameters on the coating adherence were studied. The optimal coating conditions are presented as follows: pre-oxidation of the metallic supports was performed at 900 °C for 10 h, the sol layer loadings were 2.0–6.6 wt.%, and the slurry layer loadings were less than 25.3 wt.%. The sol layer drying was performed at 30 °C for 1 h and that for the slurry layer the drying was performed at 120 °C for 2 h, and the coating calcining was performed at 900 °C for 2 h. The SEM photographs of coated samples show that alumina washcoats were well deposited on the metallic supports.