The pursuit of strong and ductile structures for cryogenic applications has fueled a persistent interest in the microstructure design of metals and alloys. While heterostructure design has recently demonstrated efficacy in achieving superior strength-ductility combinations at room temperature, its potential remains less explored in the cryogenic regime. In this report, we unveil anomalously improved cryogenic mechanical properties of a pure titanium with harmonic heterostructure that matches or even surpasses those of commercial titanium alloys. Through detailed comparison to room-temperature deformation behavior, we reveal that the superior performance of heterostructure at cryogenic temperature is fundamentally underpinned by the amplified inter-zone mechanical incompatibility and the suppression of dislocation cross-slip. The former promotes the generation of abundant geometrically necessary dislocations, and the latter optimally configures them. Collectively, these two factors culminate in the hetero-deformation-induced effect, delivering the anomalous improvement of cryogenic mechanical properties in titanium. These findings not only significantly advance our understanding of cryo-deformation behaviors in heterostructured materials but also offer the potential for developing high-performance materials for cryogenic applications.
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