A focused ion beam (FIB) technique was applied to cross-sectional specimen preparation to observe an interface between a plasma sprayed coating and an aluminum (Al) substrate by transmission electron microscopy (TEM). The surface of the sprayed coating film has a roughness of several tens of microns. Sputter rates for the coating film and the substrate are greatly different. The rough surface and the difference in sputter rate cause problems in making TEM specimens with smooth side walls. The top surface of the coating film was planerized by the FIB before fabricating the TEM specimen. The interfaces were investigated by TEM and energy-dispersive X-ray (EDX) analysis. The TEM observation revealed that there is a 10 nm thick amorphous layer at the interface between the coating film and substrate. The coating film consists of two kinds of sublayers with bright and dark contrast. The bright contrast sublayers were amorphous layers with thickness of 2~10 nm. The Al/Fe X-ray intensity ratio was larger in bright contrast sublayers than that in dark contrast sublayers.