might, however, still affect the transport of charge carriers, thereby limiting the device efficiencies. A very long electron diffusion length, greater than 175 µm, has been reported for a CH 3 NH 3 PbI 3 single crystal (SC); [7] it decreases to ≈100 nm in polycrystalline films, due to these traps. [8] Therefore, higher efficiencies are expected for PeSCs incorporating perovskite SCs. Indeed, SC perovskitebased electronic devices have attracted much attention recently. [7,[9][10][11][12][13][14][15][16][17][18] In addition to solar cells, high-performance photodetectors [14][15][16][17] and X-ray detectors [18] featuring perovskite SCs have also been demonstrated. Perovskite SCs also exhibit greater thermostability and humidity stability when compared with their thin films. As a result, the challenge remains to develop relevant technologies for synthesizing and fabricating high-quality perovskite SCs for future applications.Many approaches have been proposed for growing perovskite SCs, [19] including temperature-lowering methods, [7] antisolvent vapor-assisted crystallization, [9] and inverse temperature crystallization. [20] The fabrication of efficient solar cells from perovskite SCs has, however, been mostly unsatisfactory, due to the imbalance between the absorption length and the carrier diffusion length; the thickness of the SCs is usually too great, resulting in poor charge carrier collection efficiencies. Laterally structured CH 3 NH 3 PbI 3 SC solar cells have been constructed through piezoelectric poling, but the PCEs obtained have remained low. [10] Several methods for growing planar/thin-film perovskite SCs effectively have been demonstrated recently. [11,12,16] For example, CH 3 NH 3 PbBr 3 SCs having thicknesses ranging from one to several tens of micrometers and lateral dimensions of up to several millimeters have been grown using cavitation-triggered asymmetric crystallization (CTAC), which provides additional energy to overcome the nucleation barrier; a PCE of 6.5% has been achieved for solar cells fabricated using this method. [11] Furthermore, space-limited inverse-temperature crystallization (SLITC) has been used to grow planar CH 3 NH 3 PbBr 3 SCs having a controllable thickness of 16 µm and lateral dimensions of 6 × 8 mm; a remarkable PCE of 7.11% was reported for such a device, which also displayed excellent stability. [12] Therefore, these novel approaches can allow the preparation of perovskite SC geometries having lateral crystal structures for applications in electronic devices.The synthesis of certain perovskite single crystals (SCs), including CH 3 NH 3 PbI 3 , through asymmetric crystallization is difficult, mainly because of the large difference in solubility of the precursors and/or the intrinsic nonpreference for growth in a direction along the substrate. Herein, an effective method is reported, seeded space-limited inverse-temperature crystallization (SSLITC), for growing CH 3 NH 3 PbI 3 SC plates having micrometer-scale diameters. In this process, a seed CH 3 NH 3 PbI 3 crystal ...