Integration of aluminum (Al) and titanium (Ti) alloys offers an effective approach to sustainable and high-quality development of the automotive and aviation industries. However, challenges arise when welding Al alloys to Ti alloys due to the formation of detrimental intermetallic compounds at the interface. With the implementation of ultrasonic vibrations, the temperature and strain rate were both increased during Al/Ti friction stir welding (FSW), leading to the formation of an amorphous interlayer, instead of intermetallic compound (IMC), at the interface. The interfacial microcracks were eliminated in the ultrasonic vibrations assisted friction stir welding (UVFSW). There were Ti particles separated from the Ti substrate and dispersed in the Al alloy, thereby resulting in a more gradual and moderate evolution of the interfacial microstructure. Due to the improved interfacial microstructure with ultrasonic vibrations, the lap shear strength was almost twice that of the conventional FSW welds within same welding conditions. Meanwhile, ultrasonic vibrations also improved the fabrication efficiency with a higher optimal traversing speed. The failure mode shifted from interface separation of FSW welds to a shear dimple fracture of the UVFSW welds, demonstrating the better plasticity and reliability of the UVFSW Al/Ti dissimilar joints.