Here, the supramolecular interaction between nucleobase adenine and graphene was strengthened by a novel chemical molecular designing strategy. Based on this approach, the adenine-bridged aromatic phthalonitrile (AAPN) was prepared as stabilizer toward liquid-phase exfoliation for non-covalent functionalized graphene (AAPN-G). A series of experiments were carried out to verify the strong supramolecular interaction between AAPN and graphene. The feasibility of multifunctional application of the AAPN was briefly demonstrated. This work constitutes a feasible strategy in the preparation and functionalization of graphene that could be extended to some other (bio)molecules toward realization of designing multifunctional materials.