A superbranched multi-armed crosslinking strategy for robust conducting polymer hydrogels toward wearable sensing and encrypted communication

Conducting polymer hydrogels have attracted extensive interest in flexible electronics and wearable sensors owing to their intrinsic softness, stretchability, and biocompatibility. However, conventional hydrogel systems typically rely on linear cross-linking strategies that generate discrete junctions and topologically simple networks, limiting their mechanical robustness and functional tunability. Herein, we propose a superbranched multi-armed crosslinking strategy to construct a robust and branched architecture (RBA) conducting polymer hydrogel by integrating an amino-terminated hyperbranched polymer network (HBPN) into poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS)-based conducting polymer hydrogels. The abundant terminal amino groups in HBPN form multidirectional noncovalent interactions with hydroxyl and carboxyl groups, yielding a densely entangled and hierarchical network. The RBA conducting polymer hydrogel exhibits high stretchability (>300%) and outstanding toughness (342.76 kJ m –3 ), more than twice of its linear-cross-linked counterpart. RBA-based strain sensors deliver rapid, reversible, and stable responses with a gauge factor of 3.73, enabling precise detection of both subtle and large-scale human motions. Moreover, Morse code-based encoding system coupled with a lightweight machine-learning classifier achieves 96.26% decoding accuracy, enabling real-time assistive communication. This work offers a versatile design paradigm for conductive hydrogels toward next-generation wearable electronics and intelligent human-machine interfaces. • A superbranched crosslinking strategy was developed for robust PEDOT:PSS hydrogels. • The hydrogels exhibited excellent mechanical and electromechanical properties. • Real-time wearable sensing and encrypted communication were achieved.