In the production of value-added organics, the design of efficient photocatalysts for the selective oxidation of C-H bonds is crucial. In this work, zero-dimension (OD) Bi2MoO6 quantum dots (QDs), two-dimension (2D) g-C3N4 nanosheets (NSs), and Bi2MoO6/g-C3N4 of OD/2D heterostructure were prepared via a facile two-step process. Anchoring the Bi2MoO6 QDs on g-C3N4 NSs can shorten the charge-migration distance, extend the visible-light absorption range and provide active sites in abundance. The obtained Bi2MoO6/g-C3N4 exhibits excellent photocatalytic activity as well as stability for the selective oxidation of toluene to benzaldehyde using green O-2 as oxidant, achieving a benzaldehyde formation rate of 850.7 mu mol.g(-1).h(-1) under solvent free condition with visible light irradiation.