The spin-coating method, which is widely used for thin film device fabrication, is incapable of large-area deposition or being performed continuously. In perovskite hybrid solar cells using CH3NH3PbI3 (MAPbI3), large-area deposition is essential for their potential use in mass production. Prior to replacing all the spin-coating process for fabrication of perovskite solar cells, herein, a mesoporous TiO2 electron-collection layer is fabricated by using the electro-spray deposition (ESD) system. Moreover, impedance spectroscopy and transient photocurrent and photovoltage measurements reveal that the electro-sprayed mesoscopic TiO2 film facilitates charge collection from the perovskite. The series resistance of the perovskite solar cell is also reduced owing to the highly porous nature of, and the low density of point defects in, the film. An optimized power conversion efficiency of 15.11% is achieved under an illumination of 1 sun; this efficiency is higher than that (13.67%) of the perovskite solar cell with the conventional spin-coated TiO2 films. Furthermore, the large-area coating capability of the ESD process is verified through the coating of uniform 10 × 10 cm2 TiO2 films. This study clearly shows that ESD constitutes therefore a viable alternative for the fabrication of high-throughput, large-area perovskite solar cells.