To achieve good combination of strength and ductility, more and more attention is paid to heterostructured (HS) materials in the material community. [1,2] The microstructures of HS materials generally comprise multiple domains with remarkably different mechanical properties. The interdomain transition may be sharp or in the form of a gradient. [3][4][5] Many HS materials show better combination of strength and ductility than their homogeneous counterparts. [6][7][8][9][10] The superior properties are generally attributed to the heterozone interaction. During the loading of an HS material, the asynchronous deformation of the hard and soft domains generally causes a strong strain gradient near the interface, where geometrically necessary dislocations are accumulated to induce heterodeformationinduced (HDI) strengthening and hardening, thus contributing to achieve better strength and ductility. [11][12][13][14] Gradient materials are typical HS materials, which are characterized by a spatial gradient in the microstructure and/or composition along a certain direction. [15] In the past decades, many methods were proposed to fabricate gradient materials. Surface mechanical treatments, including surface mechanical attrition treatment (SMAT), [16] surface mechanical grinding treatment (SMGT), [17,18] and surface mechanical rolling treatment (SMRT), [19] were developed to fabricate gradient metals or alloys, with a fine grain/twin near the surface and a coarser size grain/twin in the core region. Torsion, with larger strain at the surface and smaller strain in the core of a rod, was also used to produce gradient microstructures. [20] Except for mechanical treatments, physical and chemical deposition techniques, such as electrodeposition, magnetron sputtering, and 3D printing, were developed to fabricate gradient materials. [21][22][23] By controlling the deposition kinetic and other processing parameters, such as current density, temperature, and additive content, various gradient microstructures can be tailored. In addition, laser shock peening, which applies a highenergy and ultrashort-duration laser pulse to produce a compressive shock wave and heavy plastic deformation on the surface of treated materials, was also used to prepare gradient materials. [24] Despite the aforementioned methods, it is still a challenge to fabricate bulk gradient materials with a controlled microstructure. So far, most researches have focused on materials with a gradient microstructure. A single layer of gradient microstructure was generally produced from the surface to the core region in most of the studied gradient materials. The depth or range of the gradient microstructure was limited. Few studies focus on composition-gradient materials. In natural materials, many gradient structures arose from a graded chemical composition. [25]