The as-extruded (EX) Mg-Gd-Y alloy studied here exhibited a bimodal structure, composed of fine dynamic recrystallized (DRXed) grains with random orientations and longitudinal coarse hot-worked grains. The slip analysis showed the DRXed grains exhibited mainly basal slips, while the hot-worked grains exhibited mainly prismatic slips during the tensile deformation. The distribution of geometrically necessary dislocations (GNDs) showed that there was strain partitioning between the fine and coarse grain regions. The hetero-deformation induced (HDI) hardening occurred between the two domains. It improves the strength and strain hardening capability of the alloy, leading to good strength-ductility synergy. Microcracks tended to nucleate at the DRXed grain boundaries, as well as at the interface between the two domains. The calculation of geometric compatibility parameter (m’) indicated that strain incompatibility between the adjacent grains induced the crack nucleation. The toughening effect of the fine DRXed grains hindered the crack propagation. However, the major crack formed at the interface between the two domains propagated unstably, due to the high stress concentration and the large crack size, causing the final failure.

A Mg-Gd-Y alloy prepared by surface mechanical attrition treatment (SMAT) was annealed at 450 °C combined with peak aging. The deformation and fracture mechanisms were investigated using in situ tensile tests. Through quantitative calculations of the geometrically necessary dislocation (GND) densities, it was found that the fine-grained (FG) layer in the gradient structure carried greater plastic strain than the coarse-grained (CG) layer during tension. The calculation results of the geometric compatibility parameter (m’) and microstructure characterization during in situ tests showed that crack initiation and propagation were prone to occur between adjacent coarse grains. However, the hetero-deformation-induced (HDI) strengthening and strain hardening induced by the strain gradient between the FG and CG layers effectively improved the strength–ductility synergy of the gradient-structured (GS) alloy. In addition, the synergistic effect of intrinsic and extrinsic toughening mechanisms in the GS alloy played a significant role in delaying premature failure.