Abstract Transforming potential waste materials into high-value-added sustainable materials with advanced properties is one of the key targets of the emerging green circular economy. Natural mica (muscovite) is abundant in the mining industry, which is commonly regarded as a byproduct and gangue mineral flowing to waste rock and mine tailings. Similarly, chitin is the second-most abundant biomass resource on Earth after cellulose, extracted as a byproduct from the exoskeleton of crustaceans, fungal mycelia, and mushroom wastes. In this study, exfoliated mica nanosheets were individualized using a mechanochemical process and incorporated into regenerated chitin matrix through an alkali dissolution system (KOH/urea) to result in a multifunctional, hybrid hydrogel, and film design. The hydrogels displayed a hierarchical and open nanoporous structure comprising an enhanced, load-bearing double-cross-linked polymeric chitin network strengthened by mica nanosheets possessing high stiffness after high-temperature curing, while the hybrid films (HFs) exhibited favorable UV-shielding properties, optical transparency, and dielectric properties. These hybrid designs derived from industrial residues pave the way toward sustainable applications for many future purposes, such as wearable devices and tissue engineering/drug delivery.