A dual physical crosslinking starch-based hydrogel exhibiting high strength, fatigue resistance, excellent biocompatibility, and biodegradability

Simultaneous realization of high strength, toughness, and fatigue resistance in natural starch-based hydrogel materials is challenging. A facile method of in situ self-assembly and a freeze–thaw cycle was proposed to construct double-network nanocomposite hydrogels of debranched corn starch/polyvinyl alcohol (Gels). Rheology, chemical structure, microstructure, and mechanical property of Gels were investigated. Notably, short linear starch chains were self-assembled into nanoparticles and subsequently into 3D microaggregates, which were tightly wrapped by starch and PVA network. Compared with corn starch single-network and starch/PVA double-network hydrogels, the Gels reached up to a higher compressive strength (ca. 1095.7 kPa), and then achieved to ∼20–30-fold improvement in compressive strength. Recovery efficiency exceeded 85% after 20 successive compression loading–unloading cycle tests. Furthermore, the Gels had good biocompatibility to L929 cells. Hence, the high-performance starch hydrogels are thought to serve as a biodegradable and biocompatible material to replace synthetic hydrogels, which can broaden their application fields.