Rapid Printing and Patterning of Tough, Self-Healable, and Recyclable Hydrogel Thin-Films toward Flexible Sensing Devices

Direct and rapid printing and surface patterning of hydrogel thin films are of great significance in the construction of advanced electronic devices, yet they are greatly underdeveloped due to the intrinsic contradiction between mechanical strength and self-healability as well as recyclability. Here, we present a universal and rapid slipping-directed route with a newly developed water-soluble star polymer hydrogel for direct and reproducible printing and patterning of freestanding functional thin films with precisely controlled thicknesses, components, and surface structures on a large scale. The resulting thin films combine the features of large transmittance (93%), tough mechanical strength (114 MPa), multiresponsive self-healability, recyclability, and remarkable multifunctionality. With the unique humidity-sensitive properties as motivation, diverse humidity-sensing devices including an actuating switch, a supercapacitive sensor, and a noncontact electronic skin are facilely constructed through the humidity-induced transverse, longitudinal, and patterning assembly techniques, respectively. The method presented here is universal and efficient in the fabrication and assembly of thin films with controlled configuration and functionality for advanced flexible electronics.