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Polluted water is a worldwide problem; therefore, effective separation of oil/water and removal of dyes, organic micropollutants, and heavy metals in wastewater are the need of the hour. Herein, hydrophilic β-cyclodextrin-grafted carboxymethyl cellulose, biodegradable polyvinyl alcohol, and chitosan were used as main raw materials to construct a multifunctional aerogel framework by simple sol–gel and directional freeze-drying methods. Featuring intrinsic superamphiphilic wettability in air, robust superoleophobic wettability underwater, and excellent shape-recovery characteristics, the biomass-derived aerogel presents durable oil/water separation even after 10 cycles. The aerogels possess prominent adsorption capacity for methyl blue, 1-naphthylamine, and Cu²⁺, which was as high as 121.55 mg/g, 33.96 mg/g, and 122.6 mg/g, respectively. In addition, various pollutant mixtures could be effectively adsorbed by …