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Konjac glucomannan/zeolitic imidazole framework-67 (KGM/ZIF-67) hybrid aerogels were prepared as novel adsorbents to remove malachite green (MG) from aqueous solutions. The impacts of adsorption temperature, solution pH, and ionic strength on adsorption capacity were investigated. The results show that ZIF-67 coordinates with the molecular chain of KGM and modifies the KGM aerogel. The adsorption equilibrium time of KZ2 for MG is 150 min. The adsorption process follows the pseudo-second-order and Langmuir models, with a maximum adsorption capacity of 2891.30 mg·g−1 at 30 ℃. MG adsorption using the hybrid aerogels is a spontaneous and endothermic process. This research shows that hybrid aerogels prepared using KGM and ZIF-67 are promising for use in new water purification applications. [Display omitted] • The inorganic-organic hybrid aerogels are fabricated from biopolymer-KGM and ZIF-67. • Ultra-high molecular chain of KGM perform as good carrier for the dispersion of ZIF-67 in the hybrid aerogels. • The KGM/ZIF-67 hybrid aerogels exhibit good recyclable adsorption properties for MG dye. [ABSTRACT FROM AUTHOR]