To accelerate the commercial application of organic-inorganic hybrid perovskite solar cells (PSCs), it is necessary to develop simple and low-cost methods to prepare pinhole-free large-area perovskite films with high quality. A one-step blade coating method is regarded as a scalable technique. It is demonstrated that with the addition of N,N'-dimethylpropyleneurea (DMPU) in an FA-dominated perovskite precursor, a large-area high-quality perovskite film can be obtained by blade coating, achieving improved photovoltaic performance, thermal stability, and storage stability. It is found that the strong interaction between DMPU and Pb2+ ions is beneficial to delay the nucleation crystallization process, increase the size of crystal grains, and improve the crystallinity of the perovskite film. Planar n-i-p solar cells introducing DMPU exhibit power conversion efficiencies of 20.20% for 0.16 cm2 devices and 17.71% for 5 × 5 cm2 modules with an aperture area of 10 cm2. In addition, the devices without encapsulation placed at 50 °C for 500 h and with a relative humidity of 20 ± 5% for 1000 h still maintain efficiencies above 80 and 90%, respectively, showing outstanding stability.