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Ti/Al multilayered composite, mainly composed of ultrafine equiaxed grains with a mean size of 200–300nm, has been successfully synthesized by accumulative roll bonding (ARB). The microstructure evolution and mechanical properties of the multilayered Ti/Al composite are reported. It was found that large applied shear strain, high strain rate, strain path and the low thermal conductivity of titanium are critical factors for the formation of ultrafine equiaxed grains in Ti/Al multilayered composite during the ARB process.