In this paper, hyperbranched organic montmorillonite (H-OMMT) with hydroxyl (-OH) groups was prepared. The organic montmorillonite (OMMT) was used as a reinforcing agent in NR matrix. The H-OMMT modified natural rubber (NR) had good mechanical properties with the addition of the H-OMMT. Properties, such as tensile strength and abrasion loss, were researched and compared. Results showed that NR/H-OMMT-5% composite had the best tensile and were resistant properties.