Mechanically Compatible Sealing of Hydrogel with Coherent Interface

Abstract Long‐term operation of hydrogels relies on protective coatings to avoid water swelling or evaporation, but these protections often cause substantial decreases in overall softness and stretchability. Here, a mechanically compatible seal with a coherent interfacial design is developed to encapsulate hydrogels. This seal is made from polybutylene (PIB) and polypropylene‐graft‐maleic anhydride (PP‐g‐MAH) blended poly(styrene‐isobutylene‐styrene) (SIBS). The PIB oligomers soften the SIBS networks, while the MAH groups facilitate covalent bonding between the SIBS and hydrogel. The sealed hydrogel exhibits an elastic modulus of 24 kPa and an elongation at a break of >1000%, both comparable to those of the pristine hydrogel. The adhesion energy between the seal and hydrogel reached >140 J m −2 and can be further increased to >400 J m −2 by a thermal treatment. This tough interface, together with the intrinsically low water vapor transmission rate of SIBS, allows the sealed hydrogel to maintain its modulus and stretchability after 10 days of drying in air. The sealed hydrogel is chemically and mechanically stable under harsh conditions, including acidic/alkaline/salty solutions, high temperatures, and cyclic mechanical deformation. This strategy applies to various hydrogels with diverse compositions and structures, leading to orders of magnitude improvements in the longevity of hydrogel‐based electronic devices.