A novel dual-speed tool for which the shoulder and pin rotation speeds are separately established was utilized to friction stir weld cast magnesium AZ91 with wrought aluminum 6082-T6. To assess the performance and efficacy of the dual-speed tool, baseline dissimilar welds were also fabricated using a conventional FSW tool. Optical microscopy characterized the weld microstructures, and a numerical simulation enhanced the understanding of the temperature and material flow behaviors. For both tool types, regions of the welds contained significant amounts of the AZ91 primary eutectic phase, Al12Mg17, indicating that weld zone temperatures exceeded the solidus temperature of α-Mg (470 °C). Liquation, therefore, occurred during processing with subsequent eutectic formation upon cooling below the primary eutectic temperature (437 °C). The brittle character of the eutectic phase promoted cracking in the fusion zone, and the "process window" for quality welds was narrow. For the conventional tool, offsetting to the aluminum side (advancing side) mitigated eutectic formation and improved weld quality. For the dual-speed tool, experimental trials demonstrated that separate rotation speeds for the shoulder and pin could mitigate eutectic formation and produce quality welds without an offset at relatively higher weld speeds than the conventional tool. Exploration of various weld parameters coupled with the simulation identified the bounds of a process window based on the percentage of weld cross-section exceeding the eutectic temperature and on the material flow rate at the tool trailing edge. For the dual-speed tool, a minimum flow rate of 26.0 cm3/s and a maximum percentage of the weld cross-section above the eutectic temperature of 35% produced a defect-free weld.