AbstractThe objective of this study was to obtain insight into the synthesis and structural changes of organo-montmorillonite (OMT) by tailoring montmorillonite (MMT) with the help of a quaternary ammonium salt. The OMT was prepared as a precursor to the development of enhanced asphalt rubber (AR) product. The dimethyldioctadecylammonium chloride (DDAC) provided the required thermodynamic driving force for changing the polarity of hydrophilic MMT to organophilic when both materials were mixed at 80°C under constant stirring for about 12 h. The newly synthesized OMT and base MMT were thoroughly characterized by using particle size analyzer, zeta potential, infrared (IR) spectroscopy, powder X-ray diffraction, and scanning electron microscopy (SEM) with energy-dispersive X-ray (EDX) measurements encompassing 20,936 data points. The SEM images of OMT depicted the grafted fibrils of long-chain aliphatic hydrocarbons. At the same time, EDX indicated the exchange of sodium and magnesium cations with carbon and nitrogen of the DDAC. Comparison of the IR spectra for reactants and OMT powders concluded that water molecules were removed and methyl/methylene functional groups were inserted in the OMT. The 100 basal reflections of OMT were 1.894 nm, while that of untreated MMT was 1.522 nm, which corroborated the intercalation of the long alkyl chains of the DDAC, a cationic surfactant in the OMT. The study established a simple method for the preparation of OMT to be used as an AR modifier for roadway applications supporting the utilization of nanoclay material in resolving storage stability issues and enhancing properties of recycled rubber–based asphalt products.