Fe3O4-SiO2-NH2, Fe3O4-CTABSiO(2)-NH2 and Fe3O4-SiO2-CTABSiO(2)-NH2 magnetic adsorbents were successfully prepared and could be used effectively for the adsorption of Light Green from aqueous solutions. Unlike the first sample, mesoporous silica coatings were created using cetyltrimethylammoniumbromide micelles as molecular templates on superparamagnetic iron oxide in one sample, and on silica-coated iron oxide in the other sample to improve the adsorptive properties of the nanocomposites. The characterization by FT-IR, SEM/EDX, Zeta-potential, XRD, VSM, and N-2-adsorption/desorption confirmed the production of mesoporous silica layer. Although coating processes with both silica and mesoporous silica layers led to a vaguely decrease in saturation magnetization of the Fe3O4-SiO2-CTABSiO(2)-NH2, the nanoparticles were protected with silica coatings for environment conditions and made more suitable for subsequent amino functionalization. The results determined from Batch adsorption experiments fitted to Langmuir isotherm model with maximum adsorption capacity (q(max)) equal to 56.18, 196.08 and 227.27 mg g(-1), for Fe3O4-SiO2-NH2, Fe3O4-CTABSiO(2)-NH2 and Fe3O4-SiO2-CTABSiO(2)-NH2, respectively, and it was seen from the kinetic results, the LG adsorption was identified by pseudo-second-order kinetics, revealing that LG adsorption process is homogeneous, monolayer and based on chemical interactions. According to the results, both silica and mesoporous silica coating strategy can play crucial role in improving the adsorptive properties of nanocomposites.