The hydrophilic character of palygorskite has been modified by grafting organic group and controlling surface energy for improving compatibility of palygorskite in rubber matrix using palygorskite as cis-polybutadiene rubber fillers. The effects of coupling modification on the performance of cis-polybutadiene rubber materials filled with palygorskite were investigated, and the influence of coupling agent dosage on their mechanical properties was also studied. The results indicated that the mechanical performance of cis-polybutadiene rubber materials reinforced by modified palygorskite could be improved significantly, and the tensile strength and tearing strength increased by 122.5% and 107.6% at the optimal dosage (15%) of coupling agent 3-mercaptopropyl trimethoxysilane. Moreover, the reinforcement mechanism of rubber composite materials as prepared was also analyzed. 1. Introduction cis-Polybutadiene rubber materials have the characteristics of wear resistance, excellent elastic, age resistance and so forth, and thus they have become essential in many fields [1–3]. Nevertheless, cis-polybutadiene rubber materials as organic materials could not form crystals at room temperature unless they are sufficiently stretched and have disadvantages of low compressive strength, high cost, and poor dimensional stability, and thus their stress-induced crystallization is obviously lower than that of natural rubber [4, 5]. Consequently, fillers have been widely used in rubber products, which could enhance the performance of rubber composites and reduce the production cost. The carbon black is the prime fillers in rubber industry, whose process exacerbates tensions in the energy supply and pollutes the environment. The studies on energy saving and environment-friendly fillers have focused on polymer composites along with the emphasis on the environmental protection. Natural mineral materials such as sepiolite, montmorillonite, and kaolin have been applied as fillers of polymers for various composite materials with excellent performance [6–11], because applying natural mineral materials will solve the serious environmental problem caused by carbon black production and so forth. Palygorskite is typical natural fibrillar silicate clay with large reserves in South China. The chemical structure of palygorskite is Mg5Si8O20(OH)2(H2O)4 4H2O and its smallest structure unit is fibrillar single crystal with a diameter of 20–40？nm [12–15]. Unlike the layer-layer interaction in layered silicates, the interaction between palygorskite single crystals is extremely weak due to
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