High-performance Förster resonance energy transfer (FRET)-based dye-sensitized solar cells (DSSCs) have been successfully fabricated through the optimized design of a CdSe/CdS quantum-dot (QD) donor and a dye acceptor. This simple approach enables quantum dots and dyes to simultaneously utilize the wide solar spectrum, thereby resulting in high conversion efficiency over a wide wavelength range. In addition, major parameters that affect the FRET interaction between donor and acceptor have been investigated including the fluorescent emission spectrum of QD, and the content of deposited QDs into the TiO2 matrix. By judicious control of these parameters, the FRET interaction can be readily optimized for high photovoltaic performance. In addition, the as-synthesized water-soluble quantum dots were highly dispersed in a nanoporous TiO2 matrix, thereby resulting in excellent contact between donors and acceptors. Importantly, high-performance FRET-based DSSCs can be prepared without any infrared (IR) dye synthetic procedures. This novel strategy offers great potential for applications of dye-sensitized solar cells.