Friction stir welding (FSW) technique has been successfully applied to butt joining of aluminum alloy 6061-T6 to one type of advanced high strength steel (AHSS), transformation induced plasticity (TRIP) 780/800 with the highest weld strength reaching 85% of the base aluminum alloy. Mechanical welding forces and temperature were measured under various sets of process parameters and their relationships were investigated, which also helped explain the observed macrostructure of the weld cross section. Compared with FSW of similar aluminum alloys, only one peak of axial force occurred during the plunge stage. Three failure modes were identified during tensile tests of weld specimens, which were further analyzed based on the microstructure of joint cross sections. Intermetallic compound (IMC) layer with appropriate thickness and morphology was shown to be beneficial for enhancing the strength of Al–Fe interface.