Hybrid organic/inorganic perovskite solar cells (PVSCs) are promising alternatives to traditional photovoltaic devices because of their low cost, high power conversion efficiency, and simple production process. Therefore, achieving a low-temperature and high-efficiency procedure is necessary to realize the large-scale production of PVSCs. This study developed a facile low-temperature process (70 degrees C) for the synthesis of anatase TiO2 thin films on the FTO substrate through an in situ growth method. The assynthesized anatase TiO2 thin films were applied on efficient compact layers of all low-temperature (sub-100 degrees C)-processed PVSCs. Under optimization, the achieved low-temperature PVSC device exhibited a champion conversion efficiency of up to 10.33%, with excellent repeatability and negligible hysteresis. Results revealed that fast electron extraction and transfer between perovskite and TiO2 films and effective suppression of charge recombination are the main attributes for the excellent performance of the PVSC device. This work provides a new alternative to achieve low-temperature and high-efficiency photovoltaic devices.