Simultaneous enhancement of stretchability, healability and carrier mobility in polymer semiconductors via hierarchical hydrogen-bonded engineering

Abstract Stretchable polymer semiconductors are vital for intelligent technologies such as health monitoring and human-machine interactions, suffering from a fundamental trade-off between charge transport and stretchability/self-healability. Herein, we introduce the concept of hierarchical hydrogen bonds to provide multilevel dynamic interconnected polymer network that simultaneously delivers outstanding stretchability, notable self-healing ability and high charge carrier mobility. The conjugation breaker N,N-dicarbamoylpyridine-2,6-dicarboxamide is incorporated into the polymer backbone with different strengths of hydrogen bonds, affording a crack-onset strain up to 150% and 90% mobility recovery upon healing treatment. Crucially, the hierarchical hydrogen bonds enable close interchain stacking for efficient interchain charge transport while enhancing chain dynamics and mechanical compliance. Fully stretchable transistors based on our designed polymer show stable and high mobility up to 1.01 cm2 V−1 s−1 even under 150% strain, marking unprecedented performance for healable semiconductors. Hierarchical hydrogen-bonded engineering thus establishes a design paradigm for high-performance stretchable and healable polymer semiconductors.