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In industrial applications, welding of dissimilar metals such as aluminum (Al) and titanium (Ti) is a prerequisite for the development of hybrid components with improved mechanical and corrosion properties. However, dissimilar welding of the Al/Ti system is highly challenging due to differences in the physical and thermal properties of the two materials. In the present investigation, an attempt has been made to fabricate a dissimilar friction stir weld (FSW) of commercially pure Al and Ti and to elucidate the mechanism associated with superior joint formation. The process parameters, such as tool rotation speed, traverse speed and tool offset position have been optimized using Taguchi’s optimization technique. A detailed investigation of the weld with optimum process parameters has been carried out to reveal the mechanism of joint formation. The superior mechanical properties (24% higher ultimate tensile strength and 10% higher ductility than that of base Al) of the weld are attributed to the fabrication of a defect-free joint, formation of intercalated particles and an Al/Ti interlocking interface, homogeneous distribution of fine second-phase (Ti and/or intermetallics) particles in the weld nugget, reduction in the evolution of brittle Al3Ti intermetallic compounds (IMCs) and recrystallization and grain refinement of Al in the weld nugget. The potentio-dynamic polarization test indicated that the optimized Al/Ti weld has ~47% higher corrosion resistance than Al; it had a very mild corrosion attack due to the homogeneous dispersion of fine particles. The method and mechanism could have an immense influence on any dissimilar weld and metal matrix composites, improving their mechanical properties and corrosion resistance.