A multilayered Ti-Al composite was designed and fabricated by hot pressing and hot rolling of alternately stacked Ti and Al foils. In situ electron backscatter diffraction was utilized to characterize the orientation evolution and deformed substructure upon tension. A remarkably inhomogeneous deformation mode was observed within the interior of Ti grains, in a way that the closer to the grain boundary or Ti/Al interfaces, the harder the plastic flow. Such a phenomenon is attributed to the synergetic constraint of phase interface and grain boundary. The present study thus provides a new strategy to tailor the deformation behavior of metallic materials by sufficiently leveraging the interfacial constraint effect for performance optimization.