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Polysaccharide-based hydrogel adsorbents become popular because of their high adsorption capacity and fast adsorption rate, but their low removal rate and poor pH resistance have always been fatal shortcomings. Herein, a feasible strategy was proposed to strengthen the ability of hydrogel adsorbent to remove organic pollutants (i.e., dye) by incorporating natural rectorite (REC) into chitosan- g -poly (2-acrylamido-2-methyl-propane-sulfonic-acid) hydrogel network to form a rectorite-in-polymer network structure. The introduction of less dosage of REC (1.2 wt%) into the hydrogel facilitates to improve its adsorption capacities toward methylene blue (MB) in deionized water, tap water, seawater, Yangtze River water, and Yellow River water (1083.39–1303.49 mg/g); while incorporating higher content of REC (15.8 wt% REC) helps to improve the removal rate (99.6% for MB in real waters), which are greatly superior to commercial activated carbons. The adsorbent keeps high adsorption efficiency in a broad pH range (2–11), and can be reused for >4 times. [Display omitted] • Synthesized chitosan-based hydrogel has a rectorite-in-polymer composite network. • The hydrogel shows high adsorption capacity (1303.49 mg/g) and removal rate (99.6 %). • Removal efficiency keeps high in real waters (Yangtze River, Yellow River, seawater). • The hydrogel's adsorption capacity far exceeds that of commercial activated carbon. • This method is universal to enhance the removal efficiency of hydrogel adsorbent. [ABSTRACT FROM AUTHOR]