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With the increase of sustainable development goal, the bio-based adsorption materials with high and selective dye removal are important for water treatment in the dyeing industry. In this paper, a bio-based adsorption foam composed of metal-organic frameworks (MOF) and polyethyleneimine (PEI)-modified cellulose was prepared by a three-step process, i.e., PEI modification of cellulose fibers (PC), MOF decoration of PEI-modified cellulose (MIL-53@PC), and in-situ foaming with polyurethane. PEI modification provides cellulose fiber with more active sites for both dye adsorption and MOF bonding. We found that MIL-53 crystals were tightly bonded on the surface of PC through hydrogen bonding. Because of the abundant adsorption sites (e.g., amines, iron oxide group), the MIL-53@PC demonstrated high adsorption capacity and selectivity for anionic dye (e.g., 936.5 mg/g for methyl orange) through electrostatic interaction and hydrogen bonding. Finally, MIL-53@PC particles were blended with a waterborne polyurethane prepolymer to prepare a three-dimensional hydrophilic foam (MIL-53@PC/PUF), which not only maintained high adsorption capacity and selectivity of MIL-53@PC and also improved its recyclability and reusability. The MIL-53@PC/PUF offers a promising solution for dye wastewater treatment. [Display omitted] • MIL-53@PC was fabricated via the ultrasonic method. • The maximum adsorption capacity of MIL-53@PC for MO was 936.5 mg/g. • The MIL-53@PC could selectively remove the anionic dyes from wastewater. • The MIL-53@PC/PUF broadened the practical application of powder adsorbent. [ABSTRACT FROM AUTHOR]