The preparation of poly(methacrylic acid) modified chitosan microspheres (PMAA-GLA-CTS) and its application for the removal of cationic dye, methylene blue (MB), in aqueous solution in a batch system were described. The modified chitosan was characterized using FTIR and XPS analysis. The effects of the pH of the solution, contact time, and initial dye concentration were studied. The adsorption capacity of the microspheres for MB increased significantly after the modification as a large number of carboxyl groups were introduced. The equilibrium process was better described by the Langmuir rather than the Freundlich isotherm. According to the Langmuir equation, the maximum adsorption capacity was 1 g . g(-1) for MB. Kinetic studies showed better correlation coefficients for a pseudo-second-order kinetic model, confirming that the sorption rate was controlled by a chemisorption process. Photocatalytic regeneration of spent PMAA-GLA-CTS using UV/TiO(2) is effective. Further, the regenerated PMAA-GLA-CTS exhibits 90% efficiency for a subsequent adsorption cycle with MB aqueous solutions.