This article aims to investigate the mechanical properties of the gradient structured (GS) Cu–Al–Zn alloys. To prepare the GS samples, three kinds of Cu–Al–Zn alloys with different stacking fault energies (SFEs) were processed by surface mechanical attrition treatment (SMAT) at cryogenic temperature. The results show that the Cu-5.5%Al-4.5%Zn alloy having the lowest SFE processed by SMAT for 5 min exhibits an optimized combination of strength and ductility. For both the initial annealed sample and the SMAT samples processed for the same processing time, uniform elongation (UE) and ultimate tensile strength (UTS) increase with decreasing SFE, whereas the yield strength (YS) is not sensitive to SFE. In the case of the same SFE, as the SMAT processing time increases, the YS and UTS of the GS alloy increase and the UE decrease. The optimized SMAT processing time can sufficiently refine the grains in the GS layer, which can increase the strength and maintain good ductility. Also, sufficient grain refinement promotes the better accumulation of geometrically necessary dislocations (GNDs), thus forming rather effective hetero-deformation induced (HDI) stress strengthening and HDI hardening to enhance strength while maintaining good ductility. The combination of low SFE and optimized SMAT processing time is beneficial to obtain an optimized combination of strength and ductility. Additionally, since the near-surface layer of the GS material is plastically deformed earlier than the sub-surface layer, the accumulation of GNDs at the interface between the two layers also contributes to HDI strengthening and HDI hardening to improve strength and ductility.
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