Hydrogels with excellent mechanical properties have potential for use in various fields.However, the swelling of hydrogels under water and the dehydration of hydrogels in air severelylimits the practical applications of high-strength hydrogels due to the influence of air and water onthe mechanical performance of hydrogels. In this study, we report on a kind of tough and strongnanocomposite hydrogels (NC-G gels) with both swelling-resistant and anti-dehydration propertiesvia in situ free radical copolymerization of acrylic acid (AA) and N-vinyl-2-pyrrolidone (VP) in thewater-glycerol bi-solvent solutions containing small amounts of alumina nanoparticles (Al₂O₃ NPs)as the inorganic cross-linking agents. The topotactic chelation reactions between Al₂O₃ NPs andpolymer matrix are thought to contribute to the cross-linking structure, outstanding mechanicalperformance, and swelling-resistant property of NC-G gels, whereas the strong hydrogen bondsbetween water and glycerol endow them with anti-dehydration capacity. As a result, the NC-Ggels could maintain mechanical properties comparable to other as-prepared high-strength hydrogelswhen utilized both under water and in air environments. Thus, this novel type of hydrogel wouldconsiderably enlarge the application range of hydrogel materials