Dual-Responsive Starch Hydrogels via Physicochemical Crosslinking for Wearable Pressure and Ultra-Sensitive Humidity Sensing.

Flexible hydrogel sensors demonstrate emerging applications, such as wearable electronics, soft robots, and humidity smart devices, but their further application is limited due to their single-responsive behavior and unstable, low-sensitivity signal output. This study develops a dual-responsive starch-based conductive hydrogel via a facile "one-pot" strategy, achieving mechanically robust pressure sensing and ultra-sensitive humidity detection. The starch-Poly (2,3-dihydrothieno-1,4-dioxin)-poly (styrenesulfonate) (PEDOT:PSS)-glutaraldehyde (SPG) hydrogel integrates physical entanglement and covalent crosslinking to form a porous dual-network architecture, exhibiting high compressive fracture stress (266 kPa), and stable electromechanical sensitivity (ΔI/I(0), ~2.3) with rapid response (0.1 s). In its dried state (D-SPG), the film leverages the starch's hygroscopicity for humidity sensing, detecting minute moisture changes (ΔRH = 6.6%) within 120 ms and outputting 0.4~0.5 (ΔI/I(0)) signal amplitudes. The distinct state-dependent responsiveness enables tailored applications: SPG monitors physiological motions (e.g., pulse waves and joint movements) via conformal skin attachment, while D-SPG integrated into masks quantifies respiratory intensity with 3× signal enhancement during exercise. This work pioneers a sustainable candidate for biodegradable flexible electronics, overcoming trade-off limitations between mechanical integrity, signal stability, and dual responsiveness in starch hydrogels through synergistic network design.