A novel arsenic adsorbent with hydrous cerium oxides coated on glass fiber cloth (HCO/GFC) was synthesized. The HCO/GFC adsorbents were rolled into a cartridge for arsenic removal test. Due to the large pores between the glass fibers, the arsenic polluted water can flow through easily. The arsenic removal performance was evaluated by testing the equilibrium adsorption isotherm, adsorption kinetics, and packed-bed operation. The pH effects on arsenic removal were conducted. The test results show that HCO/GFC filter has high As(V) and As(III) removal capacity even at low equilibrium concentration. The more toxic As(III) in water can be easily removed within a wide range of solution pH without pre-treatment. Arsenic contaminated ground-water from Yangzong Lake (China) was used in the column test. At typical breakthrough conditions (the empty bed contact time, EBCT = 2 min), arsenic researched breakthrough at over 24,000 bed volumes (World Health Organization (WHO) suggested that the maximum contaminant level (MCL) for arsenic in drinking water is 10 mg/L). The Ce content in the treated water was lower than 5 ppb during the column test, which showed that cerium did not leach from the HCO/GFC material into the treated water. The relationship between dosage of adsorbents and the adsorption kinetic model was also clarified, which suggested that the pseudo second order model could fit the kinetic experimental data better when the adsorbent loading was relatively low, and the pseudo first order model could fit the kinetic experimental data better when the adsorbent loading amount was relatively high.