Two‐dimensional (2D) tin (Sn)‐based perovskites have recently received increasing research attention for perovskite transistor application. Although some progress is made, Sn‐based perovskites have long suffered from easy oxidation from Sn2+ to Sn4+, leading to undesirable p‐doping and instability. In this study, it is demonstrated that surface passivation by phenethylammonium iodide (PEAI) and 4‐fluorophenethylammonium iodide (FPEAI) effectively passivates surface defects in 2D phenethylammonium tin iodide (PEA2SnI4) films, increases the grain size by surface recrystallization, and p‐dopes the PEA2SnI4 film to form a better energy‐level alignment with the electrodes and promote charge transport properties. As a result, the passivated devices exhibit better ambient and gate bias stability, improved photo‐response, and higher mobility, for example, 2.96 cm2 V−1 s−1 for the FPEAI‐passivated films—four times higher than the control film (0.76 cm2 V−1 s−1). In addition, these perovskite transistors display non‐volatile photomemory characteristics and are used as perovskite‐transistor‐based memories. Although the reduction of surface defects in perovskite films results in reduced charge retention time due to lower trap density, these passivated devices with better photoresponse and air stability show promise for future photomemory applications. Surface passivation of two‐dimensional PEA2SnI4 films with organic ligands proves to be effective in protecting the films from oxygen and moisture, and in improving the performance of the transistors. On the one hand, the degradation rate after passivation is retarded. On the other hand, passivation leads to fewer defect states and better energy‐level alignment, yielding higher mobility and light‐induced photocurrents.