Novel chitosan-based materials with a higher fatty acid glycidyl as the chemically modified agent were synthesized and the adsorption ability of the resulting polymers has been evaluated for typical anionic and cationic dyes. The successful modification was confirmed by the infrared spectroscopic measurements. As the degree of substitution was decreased, the adsorption ability of the chemically modified chitosans for anionic dyes at the higher dye concentration was increased, and the modified chitosans with a lower degree of substitution showed a higher adsorption ability than that of an activated carbon at the higher dye concentration. For cationic dyes, the chemically modified chitosan showed a good adsorption power, especially when the adsorption power was evaluated by the flow methods. The improved adsorption ability of a chemically modified chitosan material was also confirmed by comparing it with that of a crosslinked chitosan material.