Rheological and mechanical properties of polypropylene (PP)/CNCs nanocomposites were compared with those of nanocomposites containing poly(ethylene-co-vinyl alcohol) as a compatibilizer. The nanocomposites were prepared by a Brabender internal mixer at CNC contents of 5 wt%. The compression molded nanocomposite dog-bones and disks were characterized regarding their tensile and dynamic rheological behavior, respectively. The complex viscosity of the nanocomposites samples containing the compatibilizer were increased, slightly, compared to the non-compatibilized nanocomposite samples. Moreover, an overshoot in the transient start-up viscosity of the compatibilized nanocomposite was observed. The Young modulus of the nanocomposite samples containing the compatibilizer were increased up to ca. 37% compared to the neat PP. The elongation at break was decreased in all PP/CNC nanocomposite samples, but less for the nanocomposite samples containing the compatibilizer. The crystalline content of the PP in the nanocomposites and also the crystallization temperature were increased after compatibilization. These results could be ascribed to the efficiency of the poly(ethylene-co-vinyl alcohol) as a compatibilizer that favors a better dispersion and wetting of the hydrophilic CNCs within the hydrophobic PP.