Ecofriendly adsorbent materials for the rapid and efficient removal of pollutant dyes are highly desired on account of concerns about environmental pollution and human health. Herein, novel magnetic HC/Fe3O4 spherical materials have been constructed via crosslinking hydroxyethyl cellulose (HC) by poly(ethylene glycol) diglycidyl ether (PGDE) followed by the introduce of magnetic Fe3O4 by a facile and effective strategy developed in this work. The morphology, structure and magnetic behavior of the spherical materials have been systematically investigated using scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FT-IR) and vibrating sample magnetometer (VSM) techniques. Further, the spherical materials were utilized to remove congo red (CR-SO3Na) from aqueous solution under varying adsorption conditions. Meanwhile, the adsorption kinetics, thermodynamics and isothermics have been achieved to explore the adsorption process and possible adsorption mechanism of CR-SO3Na by the spherical materials. The materials show not only an efficient capacity of CR-SO3Na removal from aqueous solution, but also a sufficient magnetic property of the recovery of the materials from aqueous solution after adsorption. The spherical materials have great potential to be used as efficient adsorbents for the removal of dye-containing effluent.