high photoluminescence quantum yield (PLQY), wide wavelength tunability, and high color purity, [4][5][6] they have been attractive for light-emitting diode (LED) applications. Since the first demonstration of perovskite LEDs in 2014, [7] the device external quantum efficiency (EQE) has risen rapidly from 0.1% [7] to ≈20%, [2,4,8] and the efficiency enhancements are mainly attributed to passivation and compositional engineering, [2,8] improved charge balance by optimization of device structure, [9] and efficient light extraction. [4] More recently, these materials are considered as optical gain medium for lasers. In 2014, the first amplified spontaneous emission (ASE) was observed from CH 3 NH 3 PbI 3 thin films with a threshold of 12 µJ cm −2 and a gain of 250 cm −1 , which is ascribed to the large absorption coefficient, low bulk defect density, and slow Auger recombination rate. [10] These ASE threshold and gain values are comparable to the state of art gain media such as colloidal quantum dots [11] and organic thin films. [12] Since then, optically pumped lasers have been demonstrated based on various microcavity structures such as Fabry-Pérot cavities, [13,14] distributed feedback (DFB) gratings, [3,15] and whispering gallery cavities. [16] The flexibility of fabricating hybrid perovskite lasers using solution-processed methods enables large-scale production and is attractive for the realization of on-chip integration of photonic circuits. [17] Quasi-2D perovskites, which are also known as Ruddlesden-Popper (RP) perovskites, are mixed phases of 2D and 3D nanocrystals. In the mixture, 2D domains exhibit quantumwell-like electronic properties with strong exciton binding energy due to the reduced dimensionality. [18] Typically, the 2D perovskite (A') 2 A n−1 B n X 3n+1 domains consist of multilayers of BX 6 octahedra separated by intercalating ammonium cations A', which is too large to fit into the crystal structure and hinder the growth of 3D ABX 3 crystals (A = methylammonium (MA + ), formamidinium (FA + ), or Cs + , B = Pb 2+ , and X = I − , Br − , Cl − ). As a result, the number of layers determine the bandgap of 2D quantum-well-like domains. [19] Different from 3D perovskites, thin films of qausi-2D perovskites typically contain a mixture of domains with different layers. Within such inhomogenous Quasi-2D Ruddlesden-Popper halide perovskites with a large exciton binding energy, self-assembled quantum wells, and high quantum yield draw attention for optoelectronic device applications. Thin films of these quasi-2D perovskites consist of a mixture of domains having different dimensionality, allowing energy funneling from lower-dimensional nanosheets (high-bandgap domains) to 3D nanocrystals (low-bandgap domains). High-quality quasi-2D perovskite (PEA) 2 (FA) 3 Pb 4 Br 13 films are fabricated by solution engineering. Grazing-incidence wide-angle X-ray scattering measurements are conducted to study the crystal orientation, and transient absorption spectroscopy measurements are conducted to study the charge-carr...