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In this paper, g-C3N4-based hydrogel with a 3D network structure was synthesized via a simple and cheap reaction, using hydroxyethyl cellulose (HEC) and graphitic carbon nitride (g-C3N4) as the main materials. Electron microscope images revealed that the microstructure of g-C3N4-HEC hydrogel was rough and porous. The luxuriant scaly textures of this hydrogel were due to the uniform distribution of g-C3N4 nanoparticles. It was found that this hydrogel showed great removal ability of bisphenol A (BPA) through a synergistic effect of adsorption and photodegradation. The adsorption capacity and degradation efficiency of g-C3N4-HEC hydrogel (3%) for BPA were 8.66 mg/g and 78% under the conditions of C 0 = 9.94 mg/L and pH = 7.0, which were much higher than those for the original g-C3N4 and HEC hydrogel. In addition, g-C3N4-HEC hydrogel (3%) exhibited excellent removal efficiency (98%) of BPA (C 0 = 9.94 mg/L) in a dynamic adsorption and photodegradation system. Meanwhile, the mechanism of removal was investigated in depth. The superior batch and continuous removal capability of this g-C3N4-based hydrogel make it promising for environmental applications.