| Summary: | Bio-based hydrogels that adsorb contaminant dyes, such as methyl orange (MO), were synthesized and characterized in this study. The synthesis of poly([2-(acryloyloxy)ethyl] trimethylammonium chloride) and poly(ClAETA) hydrogels containing cellulose nanofibrillated (CNF) was carried out by free-radical polymerization based on a factorial experimental design. The hydrogels were characterized by Fourier transformed infrared spectroscopy, scanning electron microscopy, and thermogravimetry. Adsorption studies of MO were performed, varying time, pH, CNF concentration, initial dye concentration and reuse cycles, determining that when the hydrogels were reinforced with CNF, the dye removal values reached approximately 96%, and that the material was stable when the maximum swelling capacity was attained. The maximum amount of MO retained per gram of hydrogel (q = mg MO g<sup>−1</sup>) was 1379.0 mg g<sup>−1</sup> for the hydrogel containing 1% (w w<sup>−1</sup>) CNF. Furthermore, it was found that the absorption capacity of MO dye can be improved when the medium pH tends to be neutral (pH = 7.64). The obtained hydrogels can be applicable for the treatment of water containing anionic dyes.
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