Gradient-nanostructured material is an emerging category of material with spatial gradients in microstructural features. The incompatibility between gradient nanostructures (GNS) in the surface layer and coarse-grained (CG) core and their roles in extra strengthening and strain hardening have been well elucidated. Nevertheless, whether similar mechanisms exist within the GNS is not clear yet. Here, interactions between nanostructured layers constituting the GNS in a Ni alloy processed by surface mechanical rolling treatment were investigated by performing unique microtension tests on the whole GNS and three subdivided nanostructured layers at specific depths, respectively. The isolated nanograined layer at the topmost surface shows the highest strength but a brittle nature. With increasing depths, isolated layers exhibit lower strength but enhanced tensile plasticity. The GNS sample’s behavior complied more with the soft isolated layer at the inner side of GNS. Furthermore, an extra strain hardening was found in the GNS sample, leading to a greater uniform elongation (>3%) as compared to all of three constituent nanostructured layers. This extra strain hardening could be ascribed to the effects of the strain gradients arising from the incompatibility associated with the depth-dependent mechanical performance of various nanostructured layers.

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