An ovel type of quantum dot (Ph-CN) is manufactured from graphitic carbon nitride by "lining" the carbon nitride structure with phenyl groups through supramolecular preorganization. This approach requires no chemical etching or hydrothermal treatments like other competing nanoparticle syntheses and is easy and safe to use.The Ph-CN nanoparticles exhibit bright, tunable fluorescence,with ahigh quantum yield of 48.4 %i na queous colloidal suspensions.I nterestingly,t he observed Stokes shift of approximately 200 nm is higher than the maximum values reported for carbon nitride based fluorophores.T he high quantum yield and the large Stokes shift are related to the structural surface organization of the phenyl groups,w hich affects the p-electron delocalization in the conjugated carbon nitride networks and induces colloidal stability.T he remarkable performance of the Ph-CN nanoparticles in imaging is demonstrated by as imple incubation study with HeLa cells.Inthe last years,m etal-free graphene-based materials with high biocompatibility,a pparently low toxicity,a nd unique optical properties have been considered to be promising candidates to replace traditional metal-containing quantum dots in bioimaging and biomedical applications.[1] However, the large-scale chemical preparation of graphene-based nanomaterials is far from being simple and usually involves the use of corrosive and toxic agents,w hile the resulting materials exhibit relatively low photoresponse.Furthermore, the origins (quantum confinement, surface states,size effects) of the optical properties are still under debate.[2] Therefore,it is still rewarding to search for new metal-free materials with high fluorescence efficiency.Ametal-free analogue is graphitic carbon nitride with an ideal stoichiometry of C 3 N 4 ,which is set up from layered (tris-)triazine units.Graphitic carbon nitride (referred to as CN) has attracted enormous attention as ap olymeric semiconductor in photocatalysis and electrocatalysis in the last decade.[3] Nevertheless,m ost of these applications focus on the use of macroscopic materials with micrometer-sized particles,a nd the usage of nanosized CN quantum dots in bioimaging and biomedicine,for example,has been limited by their low photoluminescence (PL) quantum efficiency.[4] In the last years,several methods were successfully introduced to enhance the fluorescence efficiency. However,these methods rely on the use of concentrated acid/base processes,e tching, and/or hydro/solvothermal cutting,a nd in some cases,t he emission even fell back into the ultraviolet region.[5] Therefore,afacile,m ild, and more environmentally friendly preparation method for highly fluorescent CN is still required. Ideally,t his method should enable us to tune the PL properties (such as the Stokes shift) of the CN nanoparticles and achieve emission in the visible range.Large Stokes shifts can improve the fluorescence efficiencyowing to the drop in reabsorption events that lead to non-radiative recombination. Thus far, the maximum reported S...