In nanostructured metals, heterogeneous and hierarchical microstructures have yielded great success in improving the low ductility, which has been the Achilles heel of their application as structural materials. To achieve such microstructures, generally, current strategies focus on the design of fabrication processes rather than the application of inherently microstructural changes such as phase transition and grain growth, since they are conventionally believed as two undesirable reactions when nanostructured materials suffer instability. Here, we report a solid-reaction based technique arising from the concurrence of phase transition and grain growth, achieving a new kind of heterogeneous microstructure, i.e. dual-phase bimodal nanostructure. The physics behind the concurrence aiming to understand the dual-phase bimodal nanostructure is elucidated. The present finding, offers a feasible strategy taming, instead of inflexibly retaining, the nanostructure, which may further serve as a new guideline for alloying in designing nanostructured alloys with optimized mechanical properties and good thermal stability.