In this work, Chitosan (CS) was modified by surface grafting with poly(methyl methacrylate)(PMMA) through Michael addition method in emulsion copolymerization and then compounded with Natural Rubber (NR) latex in order to prepare PMMA-modified Chitosan/NR blends. The effect of methyl methacrylate (MMA) and chitosan concentration on the mechanical properties, morphology was investigated, and also reduced the friction of the blends by compounded molybdenum disulfide (MoS2) in order to make a bio-composites for arterial skin or others. Results showed that the Coefficient of friction was reduced obviously as the loading of MoS2 were elevated form 20 to 30 phr. And it will further cause a significant effect on the blends of Chitosan and Natural Rubber (CS/NR) Latex. Potentially it will be an important bio-material in the future. Keywords: Natural Rubber (NR), Chitosan (CS), poly(methyl methacrylate)(PMMA), molybdenum disulfide (MoS2) ,modified, friction