Crystallization and interface engineering of perovskite are the most important factors in achieving high-performance perovskite solar cells (PSCs). Herein, we construct an ultrathin CdSe quantum dots (QDs) underlayer via a solution-processable method, which acts as a seed-mediated layer for perfect perovskite film, with both uniform morphology and better absorption capacity. In addition, CdSe QDs and perovskites form a fully crystalline heterojunction, which is beneficial to minimizing the defect and trap densities. Then, an Ostwald ripening process is adopted to fabricate large-grain, pinhole-free perovskite thin film, by a simple methylammonium bromide treatment. Besides, the first principle is applied in calculating organic/inorganic hybrid perovskite, confirming that electrons can move even quicker and more effectively, as a result of our work. Due to these treatments, representing a very simple method to simultaneously control perovskite crystallization and optimize the interfaces in PSCs, a maximum power conversion efficiency of 15.68% is achieved, 35% higher than the PSC both without CdSe and MABr treatment (11.57%), indicating better performance.