Coal-based graphene sheets (GS) and coal-based graphene quantum dots (GQDs) are usually prepared separately. In this paper, symbiosis of coal-based GS and coal-based GQDs was successfully prepared with our proposed preparation method by using three raw coals with different reflectance (collected from Qinshui coalfield, Shanxi Province) as carbon sources. The results showed that coal-based GS and coal-based GQDs can exist stably in the symbiosis and are distributed in different layers, and the GQDs are freely distributed between layers of GS. The average number of GS (N
ave) in the three symbiosis is about 7 and the average interlayer spacing (d
002) is about 0.3887 nm. The average diameter of GQDs in the three symbiosis is about 4.255 nm and the average d
002 is about 0.230 nm. The average N
ave of the three symbiosis was about 3 and the average d
002 is about 0.361 nm. The morphology and crystal parameters of symbiosis is more similar to that of graphene, the elements are only carbon and oxygen. In the prepared symbiosis, the higher the reflectance of raw coal, the smoother the lattice skeleton and the less vortex-layer structure of GS, and the larger the diameter and the denser the six membered ring of GQDs. The C and O functional groups of the prepared symbionts are similar. The higher the reflectance of coal, the higher the content of C–C/C=C. Under ultraviolet light, the prepared products all emit blue, and the higher the reflectance of coal, the higher the ultraviolet absorption, and the stronger the fluorescence intensity.