Cellulose nanocrystal was modified with poly(N,N-diethylaminomethyl methacrylate) to prepare an adsorbent containing amine groups for removing anionic dyes from waste water. The prepared adsorbent was characterized by Fourier-transform infrared spectrometry (FT-IR), X-ray photoelectron spectroscopy (XPS), and thermogravimetric analysis (TGA). The adsorption was affected by various factors, such as the contact time, adsorbent dosage, dye solution pH value, initial dye concentration, and ionic strength. The results revealed that amine functional groups mainly contribute to the adsorption of azo dyes (AO7). The adsorbent showed pseudo-secondorder adsorption kinetics, indicating that the dye molecules were chemisorbed on the adsorbent. The adsorption isotherm was found to fit better with the Langmuir isotherm model than with the Freundlich isotherm model.