Adding layered double hydroxides (LDHs) to polymer compounds has been shown to make them more resistant to corrosion and improve their physical and chemical properties. However, the main challenge lies in the compatibility between inorganic LDH fillers and organic polymer matrices. The incompatibility between these two is due to differences in polarity and surface properties, which makes dispersion of LDHs within the polymer very difficult, negatively affecting the final material's performance and characteristics. In this work, Zn-Al-NO3 LDH particles were synthesized through co-precipitation method and then modified by decavanadate via the anion exchange process. Then, a silane coupling agent was used to functionalize intercalated LDH particles to make them more hydrophobic; this helped the particles to disperse well inside epoxy coating, which ultimately resulted in better corrosion inhibition performance for the coating. The concentration effect of silane coupling agent on LDHs' surface grafting was also studied using various concentrations of 3-aminopropyltriethoxy silane (APTES). Compositional and structural characterization study on revealed more insight into how the surface treatments worked. Finally, to modify LDHs, sodium dodecyl sulfate was inserted in LDH structure, then APTES molecules were grafted on the dodecyl sulfate intercalated LDHs' surface. These organic intercalation and grafting steps made LDHs more suitable with acrylic resin to form uniform composite mixture through solvent solution mixing. The thermal stability of acrylic coating improved by adding modified hybrid LDH fillers and elevation in decomposition temperature was confirmed using thermogravimetric analysis.