In this study, crosslinked poly(4-vinylpyridine/crotonic acid) [poly(4-VPy/CrA)] and its N-oxide derivative were synthesized to compare the adsorption of cationic methylene blue (MB) dye on these materials. The adsorptive removal of MB from aqueous solution onto adsorbents was studied by using column adsorption method. Experimental results showed that MB was removed more effective by poly(4-VPy/CrA)-N-oxide than poly(4-VPy/CrA) resins. The percentage removal of MB increased with pH, and it was observed that basic pH was favorable for the adsorption of MB. The adsorption capacity for poly(4-VPy/CrA)-N-oxide resin was found to 19.96 mg/g. It was found that the adsorption isotherm of the MB-fitted Langmuir-type isotherm. For the adsorption of MB, the pseudo-second-order chemical reaction kinetics provides the best correlation with the experimental data. Ten adsorption-desorption cycles demonstrated that the resins were suitable for repeated use without considerable change in adsorption capacity. © 2011 Springer-Verlag.