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Graphene manufactured by the existing method (e.g., chemical oxidation) has limitations in application due to various disadvantages. Functionalized graphic nanoplates manufactured by mechanochemical reactions can solve physical and chemical defects. So, butadiene graphitic nanoplatelets (BDGNs) are first synthesized with solid graphite and butadiene gas by using a mechanochemical reaction. The product BDGNs have outstanding properties, including very good dispersion in common organic solvents (i.e., toluene), and can be used as a reinforcing filler for poly(styrene‐co‐butadiene) (PSB) because of their chemical affinity to butadiene units. BDGN/PSB_X (BDGN loading [X] = 0.2, 0.5, 1, or 2 wt.%) nanocomposites are readily prepared using a solution process. In result, the tensile strength and Young's modulus of the BDGN/PSB_0.5 nanocomposites increased by approximately 27.9% and 81.4%, respectively, compared with those of pure PSB. Because of the efficient load transfer from the PSB to the BDGNs through the good distribution and affinity of the BDGNs in the PSB, as well as the physical cross‐linking points of the BDGNs. Therefore, a mechanochemical reaction can form in situ a variety of graphitic nanoplatelets (GnPs) without additional reaction as a filler that has remarkable affinity with various polymers, including copolymers. [ABSTRACT FROM AUTHOR]