Arsenic-contaminated water is one of the seriously environmental problems around the world. Developing arsenic removal materials have become the major focuses. Mesopaper, which is synthesized by nano-scale porous powder and paper in a sandwich structure, have been developed recently. In this study, we selected three arsenic-contaminated water samples, including two samples collected from different Chinese arsenic-endemic areas and one sample collected from Chinese Shimen realgar mine, to test its effectiveness in arsenic removal. Our findings have shown that arsenic concentrations of the three samples were significantly decreased after filter through one layer and two layers of Mesopaper. The arsenic removal efficiency for the two layers of Mesopaper was significantly higher than that shown in one layer. Additionally, the adsorbed arsenic leaching rate of nano-scale powder, which the active media for arsenic removal in Mesopaper, in different pH value solutions were all relatively low. Together, all above findings have suggested that the Mesopaper has high effectiveness in treatment of arsenic-contaminated water and without secondary arsenic pollution.