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The halloysite-iron oxide (Fe3O4–HNTs) hybrid material is prepared using a halloysite nanotube as precursor, and the Fe3O4 is immobilized on the halloysite with subsequent modification using 3-aminopropyltriethoxysilane. The influence of pH, urea hydrolysis, and the concentration of ferric chloride, polyvinyl alcohol on the synthesis of Fe3O4–HNTs hybrid materials were investigated. FT-IR was used to understand the modification of surface functionality, while the surface morphology and surface heteroatom were investigated through SEM and XPS, respectively. The phase purity of the hybrid material was studied using XRD pattern. The investigation demonstrated that the dispersion of Fe3O4–HNTs composite in epoxy resin is better than HNTs, and a significance improvement in corrosion resistance of epoxy coatings (EP) was observed. Moreover, an attempt was made to understand the mechanism of Fe3O4–HNTs/epoxy coating. [ABSTRACT FROM AUTHOR]