CdS host nanocrystals with 4.2-5.5 nm in diameter have been synthesized from air stable precursors via a synthetic chemical route and doped with rare earth (RE) terbium (Tb3+) and ytterbium (Yb3+) ions. RE3+-doped CdS cores were shelled by ZnS layers of different thicknesses. The resulting core/shell nanocrystals show a complete broadband absorption below 400-460 nm to the deep UV region depending on the size of the cores. RE3+-doped CdS nanocrystals showed a red shift in the emission as observed under irradiation of 302 nm UV light and was confirmed by room temperature photoluminescence (PL) measurements. The nanocrystals were further characterized by x-ray diffraction (XRD), transmission electron microscopy (TEM), and energy dispersive x-ray (EDX) analysis. The results show that these RE3+-doped nanocrystals can be used as solar spectral matching downconversion material to enhance photovoltaic efficiency of existing solar cells.