The yttrium metal-organic framework modified with tryptophan (NH2-Y-MOF) was integrated into a chitosan and carboxymethyl cellulose matrix using a cross-linking technique involving epichlorohydrin. The goal of the project was to develop an adsorbent that will remove trivalent arsenic (III) more effectively and structurally stabilize by having several chemically active sites. The NH2-Y-MOF/CS-CMC hydrogel beads underwent extensive property evaluation using various analytical techniques. The primary analytical techniques employed encompassed nitrogen adsorption/desorption isotherms, which were utilized to investigate the textural properties of the materials. X-ray photoelectron spectroscopy (XPS) elucidated the surface composition, while Fourier-transform infrared spectroscopy (FT-IR) enabled the identification of functional groups present. X-ray diffraction (XRD) was also applied for crystallographic analysis, and field emission scanning electron microscopy (FESEM) provided insights into the morphological characteristics of the samples. As anticipated, the NH2-Y-MOF/CS-CMC hydrogel beads demonstrated an average pore width of 1.38 nm and a specific surface area of 864.92 m²/g. The study investigated the effects of adsorption on many parameters, including dose, pH, temperature, and beginning concentration. Equilibrium and kinetic measurements assessed adsorption characteristics. The Langmuir isotherm and pseudo-second-order models adequately captured the behavior. With an adsorption energy of 30.62 kJ.mol–1, chemisorption is proposed as the primary adsorption mechanism. The increasing metal absorption with temperature indicated an endothermic and spontaneous adsorption mechanism. Arsenate As (III) adsorption ideal conditions were determined with Box-Behnken design software. Along with 0.02 g of NH2-Y-MOF/CS-CMC hydrogel beads per 25 mL of solution, a pH of 7 is advised. With a maximum adsorption capacity of 326.3 mg/g, these parameters boost the composite sponge's potential for water treatment by increasing its effectiveness in arsenate adsorption. The response surface methodology (RSM) facilitated this enhancement, optimizing results with fewer experimental trials. Examine the interaction's mechanism, which may involve complexation, electrostatic interaction, or hydrogen bonds. An evaluation of eight adsorption and desorption cycles assessed the adsorbent's reusability. Results indicated stability, with no significant decrease in removal efficiency. Its chemical composition remained unchanged pre- and post-reuse, demonstrating consistent performance and reliable structural integrity shown by X-ray diffraction data.