Tetrabromobisphenol A (TBBPA) is one most widely used brominated flame retardant worldwide. In this study, a three-dimensional alpha-Fe2O3/amino-functionalization carbon nanotube (alpha-Fe2O3/CNT-N) sponge was synthesized and applied for adsorption removal of TBBPA from aqueous solution. The maximum adsorption capacity of TBBPA on the alpha-Fe2O3/CNT-N sponge was 4135 +/- 6.09 mg.g(-1) at 303 K and pH 7.0 +/- 0.1 and the adsorption capacity was maintained in the pH range of 3-7. The adsorbed TPPBA on the alpha-Fe2O3/CNT-N sponge can be easily degraded after adding peroxymonosulfate (PMS) to generate hydroxyl and sulfate radicals. The functional groups such as -CONH2, -C=0 and pi-pi* bonds played an important role in the activation of PMS. The alpha-Fe2O3/CNT-N sponge may be considered to use for water treatment due to its good adsorption capacity, easy separation from water and simple regeneration procedures.