This study presents CdTe/CdS:Mn core–shell nanocrystals (NCs) prepared in aqueous media, using thioglycolic acid as capping agent. Firstly, CdTe NCs were synthesized, and then, Mn-doped CdS shell were deposited on the top of the CdTe core under Ar atmosphere. The NCs were structurally and optically characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), energy-dispersive X-ray (EDX), X-ray photoelectron (XPS), photoluminescence (PL), and Fourier transform infrared (FTIR) spectroscopy. The results obtained from XRD, XPS, PL, and EDX showed that the Mn ions were successfully introduced into the nanocrystalline shells. Moreover, the effect of Mn concentrations on the optical properties of the synthesized core-shell NCs was investigated. The effective band gap of the sample is in an indirect relationship with the Mn: Cd molar ratio, confirmed by PL analysis, and PL emissions can be measured at various wavelengths. The PL spectra showed 990 and 170% enhancement in the emission intensity of CdTe/CdS:Mn core/shell NCs (Mn: Cd 2.5%) compared to CdTe NCs and CdTe/CdS core/shell NCs, respectively. Consequently, the introduction of Mn dopants into the core-shell structures not only diminishes the density of quenching centers, but also reduces the effective band gap energies.