The Combination of Random Terpolymerization with In Situ Hydrogen-Bonded Engineering for Highly Stretchable Polymer Semiconductors

Stretchable polymer semiconductors are now recognized as an essential constituent for the development of forthcoming wearable technologies. Although molecular design represents a promising strategy without relying on elastomers or additives, it suffers from poor mechanical robustness with low strain tolerance, limiting the practical applications in environments subject to extreme deformation. Here, we propose a synergistic approach combining random terpolymerization with in situ hydrogen-bonded engineering to significantly improve stretchability while maintaining efficient charge transport in polymer semiconductors. The film crystallinity decreases distinctly by random terpolymerization and strain energy dissipation proceeds by hydrogen bonds, while the continual conjugation of the polymer backbone enables efficient charge transport. Our designed terpolymer semiconductor exhibits a carrier mobility exceeding 0.16 cm 2 V –1 s –1 with notable retention rates even under 200% strain in both directions, parallel or perpendicular to charge transport. Thus, this synergistic strategy provides a design paradigm to simultaneously enable excellent mechanical robustness with high charge mobility retention for polymer semiconductors.