The influence of NiCrAlY bond coating on the adhesion properties of an Fe thermal coating sprayed on an Al substrate was investigated. By applying a bond coat, an adhesion strength of 21MPa was obtained, which was higher than the 15.5MPa strength of the coating without the bond coat. Formation of cracks at the interface of the bond coat and the Al substrate was suppressed by applying the bond coat. Microstructural analysis of the coating interface using EBSD and TEM indicated that the dominant bonding mechanism was mechanical interlocking. Mechanical interlocking without crack defects in the coating interface may improve the adhesion strength of the coating. In conclusion, the use of an NiCrAlY bond coat is an effective method of improving the adhesion properties of thermal sprayed Fe coatings on Al substrates.