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To overcome the disadvantages of inhomogeneous microstructures and poor mechanical properties of additively manufactured Ti-6Al-4V alloys, a novel technique of hybrid deposition and synchronous micro-rolling is proposed. The micro-rolling leads to equiaxed prior β grains, thin discontinuous intergranular a, and equiaxed primary α, in contrast to the coarse columnar prior β grains without the application of micro-rolling. The recrystallization by micro-rolling results in discontinuous intergranular α via the mechanism of strain and interface-induced grain boundary migration. The evolution of α globularization, driven by a solute concentration gradient, starts from the sub-boundary until the formation of equiaxed primary α. Simultaneous strengthening and toughening are achieved, which means an increase in yield strength, ultimate tensile strength, fracture elongation, and work hardening rate. The formation of α recrystallization leads to more fine grain boundaries to strengthen the yield strength, and the improvement of ductility is due to the better-coordinated deformation ability of discontinuous intergranular α and equiaxed primary α. As a result, the fracture mode in micro-rolling changes from intergranular type to transgranular type. [ABSTRACT FROM AUTHOR]