Strongly luminescent CuInS2/ZnS core/shell nanocrystals were synthesized from copper iodide, indium acetate, zinc stearate, and dodecanethiol as starting compounds in octadecene solvent. The as-prepared core/shell nanocrystals exhibit a low size distribution (<10%), and present photoluminescence in the range of 550−815 nm with a maximum fluorescence quantum yield (QY) of 60%. Time-resolved fluorescence spectroscopy revealed that the lifetimes of the different spectral components are on the order of hundreds of nanoseconds, indicating that donor−acceptor pair recombinations are at the origin of the observed emission bands. The CuInS2/ZnS nanocrystals were subsequently transferred to the aqueous phase via surface ligand exchange with dihydrolipoic acid and used as fluorescent labels for in vivo imaging. After tail vein injection into nude mice, the biodistribution of the quantum dots was monitored during 24 h using fluorescence reflectance imaging.