Transforming Grain‐Boundary Brittle Precipitates to Ductility Pathways in Complex Concentrated Alloy

Conventional wisdom holds that hard grain‐boundary (GB) precipitates embrittle structural alloys by acting as crack initiation sites. In this work, we overturn this paradigm through atomic‐scale interfacial engineering, transforming brittle GB phases into ductility pathways in a machine‐learning identified model complex concentrated alloy. By precisely tailoring thermomechanical processing, we fabricated compositionally and structurally graded interfaces (GIs) that enable sequential plasticity activation and coordinated deformation across GBs. This interfacial architecture converts an intrinsically brittle multi‐phase alloy into a ductile material, achieving an exceptional yield strength of ∼1.2 GPa with a total elongation of ∼20%. The achieved strength‐ductility synergy, realized via interfacial plasticity programming, establishes a generalizable materials design strategy to overcome the persistent challenge of GB embrittlement in precipitation‐strengthened alloys.