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The pyrolysis carbon black (CBp) from waste tires accounts for more than 35% of pyrolysis products. Its poor reinforcing ability and low additional value limit heavily the wide application of thermal pyrolysis in resolving “the black pollution” problem caused by waste tires. In this study, the CBp was upgraded by hybridization with cellulose via ball milling of the CBp and microfibrillated cellulose (MFC). A series of characterizations show that the refinement of the CBp, nanofibrillation of MFC, and hybridization were simultaneously realized under the ball milling. The obtained CBp/nanocellulose hybrid (CNCH) has a bead-chain-like morphology, with the small CBp particles attached tightly to the cellulose nanofibers via hydrophobic and hydrogen-bond interactions. The aqueous suspension of CNCH was spray-dried and compounded with natural rubber (NR). CNCH showed a much higher reinforcing ability than the CBp and ball-milled CBp (mCBp), which was attributed to the unique bead-chain-like morphology, the fine dispersion of CNCH, the interlocking effect, and improved interface interaction between CNCH and NR molecular chains. Especially, NR reinforced by CNCH has very low hysteresis and higher antiabrasion ability, which means CNCH has obvious advantages to be used as reinforcing fillers in tires. The upgrading process is simple, environmentally friendly, and suitable for industrial applications. This work is expected to provide a theoretical basis and technical instruction for the use of the CBp in tires, accelerate the industrialization of pyrolysis, and resolve the black pollution problem.