The montmorillonite (MMT) functionalized by butadiene-styrene-vinylpyridine rubber (VPR) latex was prepared in aqueous solution. Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) confirmed the interactions between MMT layer and VPR to be hydrogen bond and electrovalent bond. Then, influences of VPR on the structure and properties of NR/MMT composites were investigated through swelling property representation, dynamical mechanic analysis (DMA), scanning electron microscopy (SEM) and transmission electron microscope (TEM). The results indicated the exfoliation or dispersion of MMT in NR matrix was improved significantly by adding VPR, as well as the enhanced constrained regions and rubber-filler interaction. Finally, the mechanical properties as tensile stress, tear strength of composites were promoted by 45.2%, 51.6% respectively at 8 wt% VPR loading compared to unfunctionalized composite, where the tan delta at 60 degrees C was decreased by 42.7% simultaneously that is beneficial to the development of low rolling resistance tyre.