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Steel (St) and aluminum (Al) have a high affinity to each other and form intermetallic compounds (IMCs) when bonded by friction stir welding (FSW). Understanding the effect of alloying elements of steel on the formation of IMCs will help to design joints in which the formation of IMCs is controlled. In this study, two kinds of steel, carbon steel (CS) and austenitic stainless steel (SS) with 3 mm thickness, were selected to be welded to aluminum by FSW under similar conditions. The effect of the rotation speed of the FSW tool was also examined in the range of 850–1300 RPM. The morphology, thickness, and composition of IMCs in the interfaces were studied by various characterization techniques. It was observed that the IMC layers in the SS/Al joints were much thinner than the ones in CS/Al joints (0.1–0.7 µm in SS/Al and 2–6 µm in CS/Al). Moreover, the thickness of IMC layer in CS/Al joints …