Carbon quantum dots (CQDs) are novel carbon nanomaterials and are attracting increasing interest due to their good characteristics such as hydrophilicity, chemical stability, quantum yield, small particle sizes, and low cytotoxicity. Herein, we used CQDs as stabilizers and exfoliation agents to exfoliate graphite to graphene in an aqueous medium for the first time. The functions of CQDs are to reduce the surface tension of water to match that of graphite and to make weak interactions (π-π conjugation, hydrophobic force, and the Coulomb attraction) with the graphite surface. Different characterization methods were used to evaluate the presence of layers (<5 layers) of graphene sheets with fewer defects and low oxidation. In the future, CQDs can also be good candidates to exfoliate other two-dimensional materials, such as WS2, BN, MoS2, and g-C3N4, to form two-dimensional heterostructures for a range of possible applications.