Most heavy metals are harmful to human health and the environment, even at extremely low concentrations. In natural waters, they are usually found only in trace amounts. Researchers are paying great attention to nanotechnology and nanomaterials as viable solutions to the problem of water pollution. This research focuses on the synthesis of organic thiophene derivatives that can be used as grafted ligands on the surface of silica-coated iron oxide nanoparticles to remove Cr(VI) chromium ions from water. The Vilsmeier-Haack reaction allows the formation of aldehyde groups in thiophene derivatives, and the resulting products were characterized by the FT-IR, NMR, and GC-MS. Schiff base is used as a binder between organic compounds and nanoparticles by the reaction of aldehyde groups in thiophene derivatives and amine groups on the surface of coated iron oxide nanoparticles. Schiff base functionalized FeO composites (MNPs@SiO-SB-THCA) and (MNPs@SiO-SB-THCTA) were successfully synthesized by homogeneous and heterogeneous methods and characterized by a combination of FT-IR, transmission electron microscopy, X-ray photoelectron spectroscopy, and thermogravimetric analysis. The adsorption studies, kinetic modeling, adsorption isotherms, and thermodynamics of the two materials, MNPs@SiO-SB-THCA and MNPs@SiO-SB-THCTA, were investigated for the removal of Cr(VI) from water at room temperature and at 50 mg/L. The high adsorption capacity at pH 6 for MNPs@SiO-SB-THCTA was 15.53 mg/g, and for MNPs@SiO-SB-THCA, it was 14.31 mg/g.