Flexible perovskite solar cells (FPSCs) hold great promise for lightweight and wearable photovoltaics, but improving their efficiency and durability under mechanical stress remains a key challenge. In this work, we fabricate and characterize flexible planar FPSCs on a polyethylene terephthalate (PET). A phenethylammonium iodide (PEAI) surface passivation layer is introduced on the perovskite to form a two-dimensional capping layer, and its impact on device performance and stability is systematically studied. The champion PEAI-passivated flexible device achieves a power conversion efficiency (PCE) of ~16–17%, compared to ~14% for the control device without PEAI. The improvement is primarily due to an increased open-circuit voltage and fill factor, reflecting effective surface defect passivation and improved charge carrier dynamics. Importantly, mechanical bending tests demonstrate robust flexibility: the PEAI-passivated cells retain ~85–90% of their initial efficiency after 700 bending cycles (radius ~5 mm), significantly higher than the ~70% retention of unpassivated cells. This work showcases that integrating a PEAI surface treatment with optimized electron (SnO₂) and hole (spiro-OMeTAD) transport layers (ETL and HTL) can simultaneously enhance the efficiency and mechanical durability of FPSCs. These findings pave the way for more reliable and high-performance flexible solar cells for wearable and portable energy applications.