The PL of 1L-MoS2 is demonstrated to be tuneable by laser-induced phenyl-functionalized graphene. The F-G stacked on top or bottom of MoS2 differentiate the heterostructures because the functionalization is monotopic. Moreover, we conclude that F-G does not act as one material, but is more functional, since perpendicular bound phenyl-groups are functional on their own. Thus, the MoS2 supported on top of F-G by transfer results in a 5 times enhancement of the PL intensity, since the PL signal of A 0 increases, compared to pristine G/MoS2. Consequently, the MoS2/F-G only shows PL enhancement of 1.8 times owing to the p-doping effect from phenyl-functional groups. Therefore, MoS2 supported on C-H bonds of phenyl groups instead of graphene basal plane leads to the decrease of Schottky barrier and van der Waals interaction, which is a dominating factor to enhance the PL intensity of MoS2.