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<p>Carbon-based &#8220;quantum&#8221; dots or carbon dots are surface-functionalized small carbon nanoparticles. For bright fluorescence emissions, the carbon nanoparticles may be surface-doped with an inorganic salt and then the same organic functionalization. In this study, carbon dots without and with the ZnS doping were prepared, followed by gel-column fractionation to harvest dots of 40% and 60% in fluorescence quantum yields, respectively. These highly fluorescent carbon dots were evaluated for optical imaging in mice, from which bright fluorescence images were obtained. Of particular interest was the observed competitive performance of the carbon dots <i>in vivo</i> to that of the well-established CdSe/ZnS QDs. The results suggest that carbon dots may be further developed into a new class of high-performance yet nontoxic contrast agents for optical bioimaging.</p>