Incorporating carbon nanoparticles (CNPs) into polymers can enhance their mechanical behavior; however, enhancement depends strongly on compatibility and homogeneous dispersion. Actual methods to succeed high dispersion and compatibility are complicated, have solvent‐associated problems, and long processing times. The present work proposes the increase of the dispersion and compatibility of CNPs in a polypropylene (PP) matrix to obtain a nanocomposite with high mechanical properties, using simple, fast, and green methodologies: the modification of the CNPs by cold propylene plasma and the synergistic effect resulting from mixtures of carbon nanofibers (CNFs) and graphene nanoplatelets (GNPs) with PP matrix by melt mixing. Mixtures of CNFs and GNPs in 9:1, 8:2, and 7:3 ratios at 1 and 5 wt/wt% with and without surface modification by cold propylene plasma were fabricated. The compatibility and dispersion of the CNPs in the PP matrix were analyzed by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and Raman spectroscopy, and the results were related to the mechanical properties. The results show that the use of mixtures improved the dispersion in the system and hindered the reagglomeration of CNPs, whereas surface modification with plasma promotes higher compatibility between the phases. The elastic modulus of PP reached an increase of 127.40% using a modified mixture by plasma in a 7:3 ratio (CNF:GNPs) at 5 wt/wt%, while when the CNPs were used individually, the modified CNFs and GNPs at 5 wt/wt%, reached 97.77% and 111.85%, respectively. In addition, a finite element analysis shows that the stresses in nanocomposites fabricated with mixtures of CNPs are supported to a greater extent by GNPs than CNFs due to their morphology with a low number of graphene sheets, which allows them to have greater flexibility.