The current investigation presents a green mechanochemical procedure for the synthesis of a special kind of rubber-compatible organo-montmorillonite (OMMT) for use in the inner liner compound of tires. The compatibility character of the OMMT arises from the mechanochemical reaction of the raw bentonite mineral and gum rosin as some of the organic constituents of the inner liner composition. The monitoring of OMMT synthesis by various characterization techniques reveals that gum rosin gradually intercalates into the montmorillonite (MMT) galleries during milling and increases the interlayer spacing to 41.1 ± 0.5 Å. The findings confirm the simultaneous formation of single-or few-layered OMMT platelets with average sizes from the sub-micron range up to several micrometers during the milling process. The mechanical properties of the OMMT/rubber nanocomposite, such as tensile strength, tear resistance and elongation, present a good enhancement in comparison to the un-modified material. Moreover, the organo-modification of the inner liner composition also leads to a property improvement of about 50%.