Macrogels and nanogels (5 x 6 mm and 370 nm dimensions, respectively) based on 4-vinylpyridine (p-(4VP)) were prepared using redox and microemulsion techniques. The p(4-VP)-based materials were quaternized with HCl/alkyhalides having different chain lengths to tune the charges (macro and nanogels) and size of nanogels. By developing positive charge on the p(4-VP) materials, they behaved as ion exchangers and used in removal of As(V) from aqueous environments. The prepared p(4-VP) materials were also rendered responsive to magnetic field by in situ incorporation of magnetic metal nanoparticles inside macro p(4-VP) hydrogels and by encapsulation of separately prepared magnetic ferrites by nanosized p(4-VP) particles. Nanoparticles quaternized with HCl (p(4-VP)-HCl) (1 g) removed over 95% of As(V) from a stock solution (10 mg L-1 1000 mL) in 15 min whereas bulk hydrogels removed >82% of the As(V) from an equivalent solution in similar to 12 h. Parameters effecting the As(V) removal, including pH, temperature and ionic strength, were also investigated. The synthesized magnetic p(4-VP) composites could be reused after elution with NaOH and regeneration with quaternization agents; these procedures were facilitated using an externally applied magnetic field. The Langmuir and Freundlich adsorption isotherms were also applied to study the removal of As(V) from aqueous environments. (C) 2011 Elsevier B.V. All rights reserved.