Cellulose and starch nanocrystals obtained from the acid hydrolysis of ramie fibers and waxy maize starch granules, respectively, were subjected to isocyanate-mediated reaction to graft polycaprolactone (PCL) chains with various molecular weights on their surface. Grafted nanoparticles were characterized by X-ray diffraction analysis and contact angle measurements. We observed that the nanoparticles kept their initial morphological integrity and native crystallinity. Nanocomposite films were processed from both unmodified and PCL-grafted nanoparticles and PCL as matrix using a casting/evaporation technique. We showed that mechanical properties of resulting films were notably different. Compared to unmodified nanoparticles, the grafting of PCL chains on the surface results in lower modulus values but significantly higher strain at break. This unusual behavior clearly reflects the originality of the reinforcing phenomenon of polysaccharide nanocrystals resulting from the formation of a percolating network thanks to chain entanglements and cocrystallization.
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