AbstractNanocomposites were prepared using two bioresources, viz., cellulose nanofibers (CNFs) extracted from bamboo paper-pulp waste as the reinforcing phase and natural rubber (NR) as the matrix phase. CNFs with diameters up to 50 nm were isolated from bamboo pulp waste, and nanocomposites with 5 and 10% CNFs were obtained via two-roll mill mixing of solid natural rubber with a master batch containing 20 wt% CNFs. The NR phase was cross-linked using sulphur vulcanization. The morphology studies showed that the dispersion of CNF in NR matrix was not optimal, and some aggregates were visible on the fracture surface. The tensile strength and modulus at 50% elongation increased for the nanocomposites with the addition of CNFs, accompanied by a moderate decrease in elongation at break. The storage modulus of the natural rubber significantly increased above its glass-rubber transition temperature upon nanofiber addition. The addition of CNFs also had a synergistic impact on the thermal stability of natural rubber. The susceptibility to organic solvents decreased significantly for the nanocomposites compared to crosslinked NR, which indicated restriction of polymer chain mobility in the vicinity of the nanosized CNFs in the NR matrix.