Precipitation‐Modulated Harmonic Architectures Enable Superior Strength–Ductility Synergy from Cryogenic to Elevated Temperatures in Nanostructured Alloys

ABSTRACT High‐performance materials that exhibit a robust strength–ductility synergy across cryogenic to high temperatures are essential for aerospace applications, yet achieving this combination remains a significant challenge in materials development. Here, we report that remarkable mechanical properties across a broad temperature range can be achieved in bimodal harmonic‐architectured (BHA) alloys. In this architecture, spherical precipitates stabilize coarse‐grained cores, while lamellar precipitates facilitate selective recrystallization, resulting in a reproducible necklace‐like topology. This engineered microstructure delivers exceptional mechanical performance from −196 °C to 700 °C, consistently achieving yield strengths of 1–2 GPa and ductilities exceeding 10% throughout the entire temperature spectrum. Quantitative analysis reveals that precipitation and grain‐boundary strengthening are the primary contributors to strength at all temperatures, whereas the contribution of dislocation hardening decreases progressively with increasing temperature. The deformation mechanisms exhibit temperature‐adaptive cooperation: dislocation forests and nanotwins enhance deformation at cryogenic temperatures, dislocation–precipitate interactions dominate plasticity at ambient conditions, and interfacial back‐stress accommodation ensures coordinated deformation of bimodal grains at elevated temperatures. This adaptive synergy effectively suppresses both cryogenic embrittlement and high‐temperature softening, establishing a robust structural foundation for broad service applicability. The BHA engineering offers a versatile pathway for developing next‐generation alloys with superior properties required for wide‐temperature applications.