The microstructure of the friction-bonded interface of Al alloys to low C steel has been investigated by TEM observations to reveal the controlling factor of the formation and growth of the IMC (Intermetallic Compound) layer, which caused the premature fracture at the interface even when its thickness was less than 1 μm, as reported in a previous paper. The thickness of the IMC layer observed at the interfaces of Al-Mg alloy/steel and pure-aluminum/steel joints increased almost in proportion to the friction time, but did not obey the parabolic law a characteristic kinetics of the diffusion-controlled process. Analyses of SAD patterns from the IMC layer indicate that it consisted of Fe2Al5, Fe4Al13, (Fe, Mn)Al6 and FeAl2, depending on the alloying elements. These IMCs were granular and distributed almost randomly within the IMC layer, suggesting that mechanical mixing of the steel with the Al alloy occurred at the interface. In the low C steel adjacent to the IMC layer, a zone of much finer grains than those of the base metal was observed. Its width increased with friction time and pressure, and with the growth of the IMC layer, as well. These results suggest that the superficial region of the steel underwent a heavy plastic deformation during the friction process and it had a close relation with the growth of the IMC layer.