Graphene quantum dots (GQDs), a nano version of graphene whose interesting properties that distinguish them from bulk graphene, have recently received significant scientific attention. The quantum confinement effect referring to the size-dependence of physical and chemical properties opens great possibility in the practical applications of this material. However, tuning the size of graphene quantum dots is still difficult to achieve. Here, an edge-etching mechanism which is able to tune the size of GQDs in a quasi-continuous manner is discovered. Different from the ‘unzipping’ mechanism which has been adopted to cut bulk graphitic materials into small fragments and normally cut through the basal plane along the ‘zig-zag’ direction where epoxy groups reside, the mechanism discovered in this research could gradually remove the peripheral carbon atoms of nano-scaled graphene (i.e. GQDs) due to the higher chemical reactivity of the edge carbon atoms than that of inner carbon atoms thereby tuning the size of GQDs in a quasi-continuous fashion. It enables the facile manipulate of the size and properties of GQDs through controlling merely the reaction duration. It is also believed the as discovered mechanism could be generalized for synthesizing various sizes of GQDs from other graphitic precursors (e.g. carbon fibres, carbon nanotubes, etc).