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Gradient structures ubiquitously exist in natural materials such as bone, shells, and trees. Microstructural gradients are increasingly being introduced into a wide range of engineering materials, providing them with enhanced strength, hardness, work hardening, ductility, and fatigue resistance through deformation mechanisms that are distinct from those operating in gradient-free counterparts. However, understanding structural gradient–related mechanical behaviors in all gradient structures, including those in engineering materials, has been challenging.

Although control of the structural gradient is essential to achieving optimized mechanical behaviors, existing manufacturing approaches are limiting for bulk gradient materials. For instance, surface tooling and mechanical treatments generate either limited volume fractions of gradient layers localized only near the surface or a negligible degree of …