ABSTRACTThis article presents a process for preparing organovermiculite by ball‐milling expanded vermiculite (EVMT) in water‐based ethylene vinyl acetate (EVA) latex. In this process, the vermiculite (VMT) is exfoliated to prepare a kind of EVMT/EVA modifying agent, in which EVA serves as both intercalating polymer into VMT and compatibilizer between VMT and polypropylene (PP). During melt blending between EVMT/EVA and PP, shear force exfoliates VMT sheets, dispersing them relatively well in the PP matrix. Compared with raw PP, EVMT‐modified cast polypropylene (CPP) are better when EVMT loading ranged from 0.5 to 1.0%, with improvement in both the strength and toughness of the EVMT/EVA‐modified CPP film. Specifically, tensile strength was increased by 44–54%, yield stress increased by 26%, stress at break increased by 37–43%, energy at break (toughness) increased by 29–34%, oxygen transmission rate decreased by 6.2–12.9%, the water vapor transmission rate was not significantly affected, the peel bond strength of laminated CPP film increased by 18–27%, and the processability and melt flow index (MFI) of EVMT/EVA/PP composites were improved as well. Increasing MFI attributes facilitated the processing and formation of EVMT/EVA/PP. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40954.