PSS) and CH3NH3PbIxCl3-x. In addition, perylene and perovskites form a fully crystalline heterojunction, which is beneficial for minimizing the defect and trap densities. Due to these merits, a maximum power conversion efficiency of 17.06% with improved cell stability is achieved. The finding in this work provides a simple route to control perovskite crystallizaition and to optimize the interfaces in PHJ PSCs simultaneously.