photoluminescence quantum yield, large exciton binding energy, high optical gain coefficients, and bandgap tunability. [5][6][7][8][9][10][11] Especially, the tailorable emission wavelength of perovskites is highly appealing for overcoming the so-called green gap problem in nitride-based LEDs and lasers. Since the first demonstration of amplified spontaneous emission (ASE) phenomenon of perovskites at room temperature in 2014, [5] lasering behavior has been extensively investigated for perovskite-based gain mediums combined with various optical feedback structures. [12][13][14] However, the key challenge in the practical application of 3D-perovskite is the well-known long-term instability of devices owing to atmospheric moisture and halide ion migration. [15] Recently, the solution-processed quasi-2DRuddlesden-Popper perovskites (RPPs) have been investigated as attractive alternatives to 3D-perovskites for laser applications because of their inherent stability. [16][17][18][19] The quasi-2D RPPs can be described by the chemical formula L 2 A n−1 Pb n X 3n+1 , where L represents large organic spacers such as phenylethylammonium (PEA), n-butylammonium (BA), and naphthylmethylammonium (NMA), A is a small organic cation of methylammonium (MA + ), formamidinium (FA + ), or inorganic cation of Cs + , X is a halide anion (Cl − , Br − , I − ), and n represents the number of PbX 6 octahedral layers within each period. [16] Actually, both ASE [20][21][22][23] and lasing behaviors have been widely demonstrated in the quasi-2D RPP films with whispering-gallery-mode, [24,25] Fabry-Pérot, [26,27] distributed feedback (DFB) [18,28,29] and distributed Bragg reflector [30] cavities at room temperatures. The hydrophobic bulky organic layers of cation L can suppress ion migration and prevent moisture penetration, thus imparting quasi-2D perovskites with excellent environmental and operating stability. [31][32][33][34] Indeed, it was reported that the ASE intensity maintained almost the same after excitation under continuous pulsed laser for 32 h at ambient conditions. [20] More importantly, because of dielectric constant difference between RPPs and organic layers, the excitons are confined within the [A n−1 Pb n X 3n+1 ] 2− layers, resulting in a large exciton binding energy up to hundreds of meV. [35] Furthermore, the quasi-2D RPP thin films typically consist of the mixed 2D/3D perovskite phases, naturally forming multi-quantum-well structures. Consequently, the photoexcited Solution-processed quasi-2D Ruddlesden-Popper perovskites are being considered as a promising optical gain medium in lasing applications, owing to their outstanding optoelectronic properties and inherent stability. However, the development of quasi-2D perovskites for lasers with low threshold and high optical gain is still lagging far behind 3D-perovskites. This work proposes an anti-solvent treatment strategy to regulate the phase components and surface morphology of quasi-2D PEA 2 (CsPbBr 3 ) n−1 PbBr 4 thin films. Furthermore, an additional poly(methyl meth...