In this work, the preparation, characterization and removal capability of hierarchically porous carbonaceous sponges and their g-C 3 N 4 /CS composites were described. Possessing a hierarchically porous structure and extremely large surface areas, g-C 3 N 4 /CS composites are demonstrated to have advantages in adsorption and photocatalytic activities. The adsorption and photocatalytic activities of the as-prepared catalysts were evaluated by the degradation of RhB, MO, and phenol. The best results showed that 97% decomposition of RhB was obtained by using g-C 3 N 4 /CS-60 composites within 20 min at 25°C under visible light irradiation. Furthermore, the g-C 3 N 4 / CS-60 composites showed remarkable regeneration stability, which maintains high photocatalytic activity after the samples are saturated. Additionally, the degradation mechanisms of RhB and the photocatalytic mechanism are explained in this paper.