The extraordinary mechanical performance of gradient nano-grained (GNG) structures is characterized by the heterogeneity of dislocation-based and grain boundary (GB)-based plasticity, where the grain size gradient effect on these deformation mechanisms even fracture process still remains unclear. Herein, molecular dynamics simulation is conducted on the GNG α-Fe structures to investigate the grain size gradient effect on the GB-mediated hetero-deformation mechanisms. The plastic deformation mechanism changes from GB motion (grain coarsening and merging) to GB-dislocation interaction when the grain size distribution extends from the Hall-Petch softening region to the strengthening region. With increasing grain size gradient, the ultimate tensile stress and flow stress increase in the GB motion-controlled samples, and strain partitioning between hard and soft zones is found to increase in the dislocation-GB interaction- controlled samples from an atomistic perspective. The increased strain partitioning and its accommodation process further contribute to the fracture resistance enhancement, which is demonstrated by the uniform hetero-deformation between coarse and fine grains of the GNG structure, and further avoids localized plastic deformation.
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