Biodegradable cellulose nanocrystals hydrogels (CNCsH) were synthesized from cellulose nanocrystals (CNCs) which were prepared from office wastepaper (OWP) by a chemical crosslinking method using epicholorohydrin (ECH) as a cross-linker. CNCsH were tested for their swelling behavior and biodegradability and the point of zero charge had been determined. The ability of CNCsH for removing the Acid Red 8 (AR8) anionic dye from its aqueous solution was evaluated. The different parameters affecting removal of the dye, such as pH, initial concentration of dye, content of CNCs, temperature and adsorbent dosage were investigated. The optimum conditions for 68% removal efficiency were pH = 1, initial concentration of dye = 10 ppm, contact time = 105 min, CNCs content = 5% and CNCsH dosage = 0.5 g at 30 °C. The adsorption isotherms, kinetics, and thermodynamic parameters have been studied. The results showed an appropriate fit for Langmuir adsorption isotherm and pseudo-second order kinetics model with an adsorption capacity of 17.12 mg/g. According to the obtained values of thermodynamic parameters, the removal of Acid red 8 by CNCs hydrogels was exothermic spontaneous process.