Amorphous titanium dioxide nanotube arrays (TiO2 NTs) were prepared by a simple anodization process without subsequent calcination at high temperature, and the effectiveness of amorphous TiO2 NTs as adsorbents in removing arsenite (As(III)) and arsenate (As(V)) was investigated. The TiO2 NTs were not only effective for arsenic removal without a pre-oxidation of As(III) to As(V) and/or adjusting the pH value of water before the adsorption process, but also can be separated and recovered easily from the solution. The adsorption kinetics and adsorption capacity of the amorphous TiO2 NTs for As(III) and As(V) were studied separately by batch experiments. The apparent values for Langmuir monolayer sorption capacities were 28.9 mg/g for As(III) and 24.7 mg/g for As(V) at pH 7. Kinetics studies indicated that the adsorption process on TiO2 NTs followed a pseudo-second-order kinetics model. Arsenic adsorption of TiO2 NTs remains stable over a broad pH range. Moreover, the TiO2 NTs have excellent stability and regeneration, and they can be used repeatedly at least five times.