Owing to the poor light absorption and restricted charge transport of two-dimensional (2D) perovskites, their application as photovoltaic materials is limited, and 2D perovskite solar cells (PSCs) show inferior efficiencies. Moreover, due to rapid crystallization, the quality of 2D perovskite films is often bad. To address these challenges, a strategy is proposed here for developing a high-quality patterned 2D perovskite with regularly arranged cylinder patterns for use in efficient PSCs. In the patterned imprint process, the recrystallization of the 2D perovskite occurred under the template with directional compressive stress. In this case, the oriented growth of the crystal, especially the 3D-like phase inside, was promoted. This led to a film with much higher quality, fewer defects, and optimized crystal quality, facilitating charge transfer. In particular, regularly arranged cylinder patterns were favorable for improving light absorption and increasing interfacial contact. Eventually, the PSCs based on the patterned 2D perovskite film exhibited improved power conversion efficiencies of up to 18.10% and improved general stability under different conditions. In light of the above, the patterned imprint is considered a scientific technology for the production of high-quality 2D perovskite films.