A novel TiO 2 hydrogel cage model was built for the removal of methylene blue (MB), an organic pollutant. This TiO 2 hydrogel cage was prepared with the biomass materials of hydroxyethyl cellulose (HEC) and carboxymethyl cellulose (CMC), and this hydrogel cage structure was characterized by scanning electron microscopy, transmission electron microscopy, and X-ray diffraction. The contents of the encased TiO 2 and its swelling properties with different CMC proportions of this hydrogel cage were studied to obtain a suitable crosslinking network structure and optimal synthesis conditions. Compared to an equivalent amount of pure TiO 2 , the much higher removal efficiency of MB with our prepared TiO 2 hydrogel cage was attributed to the synergistic effect of the photocatalytic degradation for TiO 2 and the adsorption enrichment for cellulose hydrogels. Furthermore, the adsorption kinetics of the intraparticle diffusion model were used to study the adsorption enrichment process of the TiO 2 hydrogel cage. In addition, on the basis of the results of photocatalytic degradation and recycling experiments, excellent performances with respect to self-cleaning, regenerative ability, and easy recovery, were shown for this HEC-TiO 2 -CMC cage material, which demonstrated ideal application potential for MB removal.