Highly Stretchable Sensitive Multiscale Hydrogel Inspired by Biological Muscles for Wearing Sensors

Hydrogels have attracted substantial research interest for application in wearable electronics due to their stretchability, elasticity, and compliance. However, most hydrogels could not satisfy the application requirements for high-performance wearable sensors due to their poor sensitivity, low mechanical properties, and sensing detection range until this day. Inspired by the fascia in biological muscles, we propose a strategy to form entangled "clusters" through the dense entanglement between highly cross-linked elastic hydrogel microspheres and polymer segments, and prepared a multiscale hydrogel with high sensitivity and mechanical toughness. This strategy embedded highly swollen hydrogel microspheres (with different pore sizes) to act as the microregions of dense entanglement in the soft matrix to adjust the microstructure of multiscale gel. When pressure was applied, this structure could provide a fast response due to the stack layer formed by microspheres and soft matrix produced effective stress distribution, resulting in the outstanding sensitivity of the multiscale hydrogel (S = 1.1 kPa^-1) in the pressure range of 0-50 kPa. The distinct microspheres functioning as microscale joint areas significantly augment energy dissipation, culminating in exceptional mechanical stability, ultrastretchability (≈1050%), and high strength of the multiscale hydrogel. The most notable progress was that the synthesized multiscale hydrogel not only combined the above advantages but also simultaneously solved multiple dilemmas of tedious synthesis steps, high cost, and poor durability. Besides, the multiscale hydrogel also had excellent antibacterial properties and biocompatibility, which enabled them to have large-scale application potential in wearable and implantable electronic devices. Our research could provide a universal approach to the creation of robust, flexible, wearable, and sensitive sensors, significantly increasing the uses of stress sensors in wearable technology.