Colloidal upconversion (UC) nanocrystals were explored as energy relay materials for dye-sensitized solar cells for the first time. The utilization of colloidal UC nanocrystals was found to significantly enhance the upconversion efficiency and improve the photocurrent of the cells for low infrared irradiation intensity. In addition, it was found that UC nanocrystals of small size favor infiltration into a TiO2 film and bring higher relay efficiency. Finally, we found that UC nanocrystals can serve as a scattering material to increase the light absorption capability of the cells and increase the overall photocurrent of the cells under simulated sunlight irradiation.