CdSe and CdTe nanocrystals are linked to nanostructured TiO2 films using 3-mercaptopropionic acid as a linker molecule for establishing the mechanistic aspects of interfacial charge transfer processes. Both these quantum dots are energetically capable of sensitizing TiO2 films and generating photocurrents in quantum dot solar cells. These two semiconductor nanocrystals exhibit markedly different external quantum efficiencies ( approximately 70% for CdSe and approximately 0.1% for CdTe at 555 nm). Although CdTe with a more favorable conduction band energy (E(CB) = -1.0 V vs NHE) is capable of injecting electrons into TiO2 faster than CdSe (E(CB) = -0.6 V vs NHE), hole scavenging by a sulfide redox couple remains a major bottleneck. The sulfide ions dissolved in aqueous solutions are capable of scavenging photogenerated holes in photoirradiated CdSe system but not in CdTe. The anodic corrosion and exchange of Te with S dominate the charge transfer at the CdTe interface. Factors that dictate the efficiency and photostability of CdSe and CdTe quantum dots are discussed.