The inevitable oxidation of Sn 2+ and p-type self-doping has plagued the development of two-dimensional (2D) Snbased perovskite field effect transistors. In this work, we demonstrate the modulation of the properties of phenethylammonium tin iodide ((PEA) 2 SnI 4 ) perovskite thin films by introducing the aromatic polymer additives of poly(4-vinylphenol) (PVP) and poly(vinyl pyrrolidone) (PVPD) during the crystallization processes, keeping the 2D layered structure of (PEA) 2 SnI 4 unchanged. The proposed formation mechanisms of the polymer-assisted (PEA) 2 SnI 4 :PVP and (PEA) 2 SnI 4 :PVPD films disclose that the interactions between the polymers and (PEA) 2 SnI 4 , such as hydrogen bonds, π−π interactions, and coordination bonds, lead to the improvement of the morphology and crystallization as well as the inhibition of Sn 2+ oxidation of the films. However, the field-effect transistors based on the two polymer-assisted (PEA) 2 SnI 4 thin films constructed on the dielectric of poly(vinyl alcohol) (PVA) modified by crosslinking PVP (CL-PVP) exhibit quite a different performance. Compared with the (PEA) 2 SnI 4 transistor, without sacrificing the hole mobility, the on−off current ratio of the (PEA) 2 SnI 4 :PVP device increases by one order of magnitude, and the subthreshold slope declines slightly due to the reduced leakage current, which results from the reduction of p-type self-doping of the perovskite film and the improved quality of the perovskite/dielectric interface because of the strong π−π interactions between the benzene rings in CL-PVP and (PEA) 2 SnI 4 :PVP. In contrast, the (PEA) 2 SnI 4 :PVPD transistor exhibits relatively poor overall performance because of the N-vinylpyrrolidone of PVPD. More importantly, employing PVP and PVPD as additives can effectively enhance the chemical stability of (PEA) 2 SnI 4 as well as the operational stabilities of the corresponding transistors. Our work provides an effective strategy for selecting chemical additives to improve 2D perovskite properties and suppress the oxidation of Sn-based perovskites, and paves a way toward the future applications of Sn-based perovskite optoelectronic devices with high performance and stability. KEYWORDS: (PEA) 2 SnI 4 , 2D layered structure, aromatic polymer additives, interactions, field-effect transistors