This study evaluated the effectiveness of a novel adsorbent (Fe(III)-AM-PGMACell), Iron(III)-coordinated amino-functionalized poly(glycidyl methacrylate)-grafted cellulose for the adsorption of arsenic(V) from aqueous solutions. The Fe(III)-AM-PGMACell was prepared through graft copolymerization of glycidyl methacrylate (GMA) onto cellulose (Cell) in the presence of N,N′-methylenebisacrylamide (MBA) as a cross linker using benzoyl peroxide initiator, followed by treatment with ethylenediamine and ferric chloride in the presence of HCl. Batch experiments were performed to evaluate the adsorption efficiency of Fe(III)-AM-PGMACell towards As(V) ions. The contact time to attain equilibrium and the optimum pH were 90 min and 6.0, respectively. More than 99.0% adsorption was achieved from an initial concentration of 25.0 mg/L. A two-step pseudo-first-order kinetic model agreed well with the dynamic behavior for the adsorption process. Equilibrium data fitted well with Sips isotherm model with maximum adsorption capacity of 78.8 mg/g at 30°C. The desorption of As(V) was achieved over 98.0% with 0.1 M NaCl solution.