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This work prepared a double-cross-linked biohybrid aerogel (DCBA) bead biosorbent from waste bamboo paper and chitosan by sequential physical (hydrogen bonding and electrostatic interaction between -COO^- and -NH₃⁺ groups) and chemical (polymerization reaction between -COOH and -NH₂, dehydration condensation between Si-OH and -OH) cross-linkings. The resulting DCBA bead was applied to remove cationic (Methylene blue, MB) and anionic (Congo red, CR) dyes in both single and binary systems. The MB and CR adsorption capacities of DCBA bead increased with increasing adsorbent dosage, contact time, temperature and initial dye concentration. With increasing solution pH, the MB adsorption capacity increased, while that for CR increased first and then decreased. The maximal adsorption capacities for MB and CR were 653.3 and 559.6 mg/g, respectively, in the single system. The …