3D metal halide perovskites take on the form ABX 3 , in which A is typically either a small organic cation such as methylammonium or formamidinium or an inorganic cation such as cesium, B is a divalent metal, and the X-site is occupied by a halide ion. Following the success of these 3D metal halide perovskites, attention has recently (re)turned to their lowdimensional counterparts as a promising class of materials for a variety of optoelectronic applications. [1] Most notable of these are the layered metal halide compounds that take on the form A 2 BX 4. In these perovskitelike structures, layers of inorganic octahedra are separated by relatively large organic cations that act as an insulating barrier, thereby forming a natural quantum-well structure. [2,3] By adjusting the thickness or composition of the inorganic layer or organic cations, fundamental material parameters such as the bandgap, effective mass, and exciton binding energy can be tuned to cover a wide range of values. [4] The strong quantum and dielectric confinement in these layered 2D perovskites generally give rise to narrow excitonic luminescence spectra that make these materials particularly attractive candidates for the fabrication of color-pure light-emitting diodes and lasers. [5-8] In addition, despite their large exciton binding energies, 2D perovskites are also increasingly used in solar cells where the addition of small quantities of 2D perovskites is found to increase the thermal and ambient stability as well as the crystallinity of the 3D perovskite film.