Mechanically Adaptive Polymers Constructed from Dynamic Coordination Equilibria

Abstract Designing materials capable of adapting their mechanical properties in response to external stimuli is the key to preventing failure and extending their service life. However, existing mechanically adaptive polymers are hindered by limitations such as inadequate load‐bearing capacity, difficulty in achieving reversible changes, high cost, and a lack of multiple responsiveness. Herein, we address these challenges using dynamic coordination bonds. A new type of mechanically adaptive material with both rate‐ and temperature‐responsiveness was developed. Owing to the stimuli‐responsiveness of the coordination equilibria, the prepared polymers, PBMBD‐Fe and PBMBD‐Co, exhibit mechanically adaptive properties, including temperature‐sensitive strength modulation and rate‐dependent impact hardening. Benefitting from the dynamic nature of the coordination bonds, the polymers exhibited impressive energy dissipation, damping capacity (loss factors of 1.15 and 2.09 at 1.0 Hz), self‐healing, and 3D printing abilities, offering durable and customizable impact resistance and protective performance. The development of impact‐resistant materials with comprehensive properties has potential applications in the sustainable and intelligent protection fields.