Cellulose nanoparticles (CelNPs) prepared by an acid hydrolysis process were acetylated under ambient conditions to retain the nanosize and to obtain hydrophobic nanosized derivatives. Green nanocomposites of natural rubber (NR) with more than 50 phr of cellulosic fillers were successfully developed by a commercial dry mixing process. The incorporation of cellulose acetate nanofiller up to 40 phr led to an almost linear increase in both the tensile and elongation properties, which were higher than even those of a composite with the conventional filler carbon black (CB). This was further supported by the almost uniform single‐phase morphology of the nanobiocomposite revealed by scanning electron microscopy and the high thermal stability. The results indicate the high degree of compatibility between the hydrophobic nanosized filler and the NR matrix. Although a drop in the mechanical strength was observed above 50 phr, the cellulose derivatives were expected to prove to be promising substitutes for the hazardous filler CB even at higher loadings. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40632.