An Asymmetric Glassy Wrinkled Hydrogel for Integrated Antifouling Protection and Robust Adhesion

ABSTRACT The pervasive challenge of surface fouling accelerates material degradation and functional failures across diverse applications, from marine infrastructure to biomedical implants and wearable electronics. A critical yet unmet need is the integration of durable antifouling capability and robust substrate adhesion within a single material. Here, we report an asymmetric hydrogel designed to address this challenge. Through the synergistic combination of gradient coordination crosslinking and non‑uniform strain recovery, we engineer a monolithic hydrogel featuring a rigid, glassy wrinkled upper layer and a soft, rubbery smooth lower layer. This architectural dichotomy yields spatially decoupled yet complementary functionalities: the upper layer achieves a high Young's modulus of 510 MPa and enables ultrafast anisotropic liquid transport, while the lower layer maintains a low modulus (∼0.2 MPa) and delivers strong, broad‑spectrum adhesion to various substrates. When conformally adhered to target surfaces, the wrinkled hydrogel efficiently removes both oily and particulate contaminants, with its glassy microstructure retaining structural and functional integrity over 200 repeated cleaning cycles, demonstrating outstanding operational durability. This work establishes a scalable fabrication strategy that enables synergistic heterofunctional integration across two opposing surfaces of a single hydrogel, providing a versatile design paradigm for advanced, long‑lasting antifouling protection systems.