High-temperature colloidal synthesis of InAs/InP and InAs/CdSe core/shell nanocrystal quantum dots is reported. InP and CdSe shells with several thicknesses were grown on InAs cores ranging in diameter between 20 to 50 Å. Optical spectra, X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and X-ray diffraction (XRD) were used to analyze the core/shell quantum dots and determine their chemical composition, average size, size distributions, and structures. The experimental results indicate that shell growth is uniform, expitaxial, and controllable. For both InP and CdSe shells, growth is accompanied by a red shift of the band gap energy as a result of the extension of the electron wavefunction into the shell region. An increase of the room temperature photoluminescence quantum yield by a factor of∼4 is observed with CdSe shell growth on InAs Cores. The growth of InP shells, however, quenches the photoluminescence quantum yield. The difference is assigned to outer surface effects in core/shell nanocrystals.