The synthesis and photoluminescence (PL) properties of aqueous CdTe/ZnO core/shell quantum dots (QDs) have been investigated by using thiolglycolic acid as a capping reagent. The highlighted contribution of the present study was CdTe QDs coated with a ZnO shell by controlling the hydrolysis process of Zn(OAc)(2). The QDs benefitted from overcoming the high lattice mismatch between CdTe and ZnO. The PL peak wavelength of the CdTe/ZnO QDs with high PL quantum yields up to 88% was located in a range between 547 and 596 nm by adjusting the size of CdTe cores and the thickness of ZnO shells. The results of X-ray diffraction analysis and transmission electron microscopy observation indicate that the dot-shaped CdTe/ZnO QDs (566 nm) with an average size of 2.2 nm in diameter belong to the cubic CdTe crystal structure. Due to the passivation of surface defects, it is found that the luminescence decay curves accord with a biexponential decay model of exciton and trap radiation behavior. The average PL lifetimes of CdTe (571 nm) and CdTe/ZnO (596 nm) QDs at room temperature are 27.3 and 35.1 ns, respectively.