Carbon-based “quantum” dots (or “carbon dots”) are generally defined as surface-passivated small carbon nanoparticles that are brightly fluorescent. Apparently, the carbon particle surface passivation in carbon dots is critical to their fluorescence performance. An effective way to improve the surface passivation is to dope the surface of the precursor carbon nanoparticles with an inorganic salt, followed by the typical functionalization with organic molecules. In this work we passivated small carbon nanoparticles by a combination of the surface-doping with nanoscale semiconductors and the organic functionalization, coupled with gel column fractionation to harvest the most fluorescent carbon dots, which exhibited fluorescence emission quantum yields of up to 78%. Experimental and mechanistic issues relevant to potentially further improve the performance of carbon dots toward their being quantitatively fluorescent are discussed.