Stretching‐Orientation Reinforced Double Network Solvent‐Free Eutectic Gels for Ultrarobust, Flexible Human‐Machine Interaction Devices

Abstract Conductive gels hold promise for human‐machine interaction (HMI) devices but face limitations in brittleness, solvent reliance, and fatigue resistance. These challenges are addressed by designing a solvent‐free, stretch‐oriented double‐network eutectogel integrating high‐molecular‐weight polyacrylamide (structural reinforcement) with a dynamic poly(acrylic acid)/choline chloride deep eutectic network (ionic conductivity). Synergistic effects between molecular chain entanglements and stretch‐induced alignment enhance mechanical robustness and energy dissipation, achieving tensile strength of 30.70 MPa, elongation of 703%, and record‐high toughness of 133.86 MJ m ⁻³ (surpassing reported eutectogels). Crucially, the aligned microstructure preserves conductive pathways, enabling multimodal sensing with high sensitivity ( GF = 1.4 at 250% strain; TCR = 14.7% °C ⁻¹ ) and stability (>300 cycles, without abrupt signal drift). Solution‐based processing compatibility facilitates scalable fabrication of ultrathin coatings and printed patterns, demonstrated in functional HMI devices: a somatosensory glove (joint motion accuracy, latency <17 ms), and capacitive touchscreens (latency <34 ms), and temperature sensors (high thermal resolution). By resolving the strength‐flexibility paradox, this work provides a platform for wearable HMI systems requiring transparency, ultrahigh strength, intrinsic flexibility, and environmental adaptability.