The well-known advantages of OSCs over their inorganic counterparts lie essentially in their relatively high absorption coefficient (α ≈ 10 5 cm −1 ) and photoluminescence (PL) quantum yield, as well as their high solution processability, which reduces device fabrication costs. [4][5][6] All these properties could be further tuned and optimized by rational structure design and chemical synthesis, which have permitted extensive utilization of OSCs as active materials in organic solar cells [7][8][9] and light-emitting diodes (LEDs), [10][11][12] as well as efficient optical gain media in organic lasers. [13][14][15] Large polycyclic aromatic hydrocarbons (PAHs) have emerged in recent decades as unique OSCs with promising optical properties and high chemical and photostability. [16][17][18][19][20][21] These large PAHs, having discrete quasi-zero-dimensional graphene structures, can also be regarded as graphene quantum dots (GQDs). [22][23][24][25][26][27] In contrast to zero-bandgap graphene, the quantum confinement of the wave function in GQDs permits the opening of a finite energy gap, conferring appealing features that can be exploited in optoelectronics and photonics, such as a relatively large Frenkel exciton binding energy [28] and multicolor fluorescence. [29][30][31][32] In the fields of Materials Sciences, GQDs are