CdSe-sensitized heterojunction solar cells composed of mesoscopic TiO 2 /CdSe/P3HT (poly-3-hexylthiophene) were constructed, and the negative molecular dipole of 4-methoxybenzenethiol (MBT) and the ZnS passivation layer were used as interface modifiers to improve device performance. Through the interface modification between TiO 2 /CdSe and P3HT using MBT and by ZnS surface passivation, the power conversion efficiency of the modified solar cell was greatly enhanced from 1.02% to 1.62% under 1 sun illumination.