The poly(4-vinylpyridine)-graphene oxide-Fe3O4 magnetic nanohybrid (GO-Fe3O4@P4VP) was prepared and used as a novel nanoadsorbent to efficiently remove methyl blue (MB) from aqueous solution. The GO-Fe3O4@P4VP was characterized with scanning electron microscopy, transmission electron microscopy, elemental analysis, BET surface area, X-ray diffraction, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy and vibrating sample magnetometer. The GO-Fe3O4@P4VP had high surface area, porous structure and magnetic properties. Adsorption performances of GO-Fe3O4@P4VP for MB were investigated at different pH, initial concentrations of MB, ionic strength, adsorbent dosage, contact time and the temperature. Adsorption equilibrium and kinetic process of MB on GO-Fe3O4@P4VP were well described by the Freundlich isotherm model and the pseudo-second-order kinetic model, respectively. Additionally, the characteristics of high adsorption capacity, rapid adsorption rate, good reusability and magnetic separation would make GO-Fe3O4@P4VP become a perfect candidate to remove MB in aqueous solution.