Two-dimensional materials with van der Waals structure attract intense interest due to their high performance in ultrathin optoelectronic devices. In particular, the high efficiency charge separation between the two-dimensional materials can significantly improve the photo-response of a given device. Here we report the discovery of pure ultraviolet (UV) emission from few layer graphene nanosheets (GNS). Near unity charge separation efficiency is key to pure UV emission. The dynamics of an excited electron were analyzed using femtosecond transient absorption techniques. Electron transfer is observed from surface defect states induced by oxygen-containing functional groups to intrinsic sp2 domain states in few layer GNS. Moreover, a solar blind response device based on few layer GNS with a high on-off ratio was successfully fabricated.