Quadruple Hydrogen‐Bonds Engineering for Intrinsically Stretchable and Healable Semiconducting Polymers

Developing intrinsically stretchable and healable semiconducting polymers with high charge-carrier mobility is critical for next-generation flexible electronics; however, integrating these conflicting functionalities remains a formidable challenge. Here, we report a "quadruple-hydrogen-bonds end-capping" strategy to realize high-performance stretchable and healable semiconducting polymers. By incorporating quadruple hydrogen-bonds between end-capping units linked with alkyl spacers into polymer backbone, we engineer a supramolecular architecture that achieves enhanced crystallinity and improved ordered packing with reduced π-π stacking distance, and also superior stretchabillity with molecular-ordering retention during stretching. Moreover, enhanced chain mobility together with dynamic and reversible and hydrogen-bonding sites in the architecture contribute to efficient healing. Consequently, our designed semiconducting polymer exhibits a more than 2-fold increase in mobility, while demonstrating stable mobility retention under strain, high mobility recovery after healing, and scalability in fully stretchable transistor arrays. This work provides an effective molecular design strategy for achieving simultaneous improvements in electrical performance, mechanical stretchability, and healing ability in organic electronics.