In this work, the Argon (Ar) plasma technology is adopted for pyrolytic carbon black (CBp) modification and the N330/Modified‐CBp (MCBp) hybrid is then incorporated into the Natural Rubber (NR) matrix. Compared with CBp, the MCBp has smaller particle size, lower ash content, higher specific surface area, and surface activity based on the results of laser diffraction method, transmission electron microscope (TEM), thermogravimetric analysis, gas sorption analysis (Nitrogen), acetone solvent, and X‐ray photoelectron spectroscopy. Among them, Dv (90) is found to have reduced by 20% while the specific surface area increased by 4%. According to the bound rubber content experiments, the equilibrium swelling experiments as well as the temperature and strain sweeps, the bound rubber content, filler‐filler bond strength, and cross‐linking density of NR/N330/MCBp are all superior to those of NR/N330/CBp, resulting in an outstanding comprehensive performance of NR/N330/MCBp composite. In particular, the 300% modulus and the tear strength rise by 43% and 14% respectively, surpassing even the system filled with N330. Finally, the mechanism of mechanical properties improvement in the NR/N330/MCBp composite is proposed: the strong filler‐filler bond is formed between the MCBp and N330 aggregates via molecular chains, and they are anchored on the MCBp and absorbed on the N330 simultaneously.