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The copper harmonic structure, which consists of a coarse-grained "core" surrounded by a three-dimensional continuously connected fine-grained "shell," exhibits both high ductility and high strength. In the present study, dislocation interactions at the shell–core boundary in the copper harmonic structure were directly measured using nanoindentation and microstructural observations via kernel average misorientation (KAM) to further understand the reason for its excellent mechanical properties. KAM analysis showed that the dislocation density in the vicinity of the shell–core boundary within the core region gradually increases with increasing plastic strain. The variation in the nanohardness exactly corresponds to the KAM, indicating that the higher strength is primarily caused by the higher dislocation density. The critical load for nanoindentation-induced plasticity initiation was lower at the shell–core boundary than at the core–core boundary, indicating a higher potency of dislocation emission at the shell–core boundary. Because dislocation–dislocation interactions are one of the major causes of the increase in the flow stress leading to higher strain hardening rates during deformation, the excellent balance between strength and ductility is attributed to the higher potency of dislocation emission at the shell–core boundary. [ABSTRACT FROM AUTHOR]