A series of sensitized TiO 2 NPs with enhanced photocatalytic activity were prepared by different sized CdTe QDs with bifunctional ligand interlinking. The microstructures and morphologies of four different sizes of CdTe QDs and CdTe QDs sensitized TiO 2 NPs were characterized systematically by fluorescence spectroscopy, UV-Vis diffuse reflectance spectroscopy, FT-IR, XRD, XPS, FE-SEM, HRTEM, BET, and positron annihilation lifetime spectroscopy (PALS). The photocatalytic performance of CdTe QDs sensitized TiO 2 NPs was investigated by degrading MO and MB in aqueous solution under visible light irradiation. The process of degradation complied with the firstorder reaction kinetics. Four different sized CdTe QDs sensitized TiO 2 exhibitedhigher photocatalytic activities than TiO 2 . Particularly, yellow emitting CdTe QDs (3.28 nm) sensitized TiO 2 (CT_1.5) showed the best photocatalytic performance, which may be attributed to the optimal NP size, and has a moderate light absorption and electron injection. The effect of microstructural defects on CdTe QDs sensitized TiO 2 has been confirmed effectively by positron lifetime measurements.