Abstract Directly growing perovskite single crystals on charge carrier transport layers will unravel a promising route for the development of emerging optoelectronic devices. Herein, in situ growth of high‐quality all‐inorganic perovskite (CsPbBr3) single crystal arrays (PeSCAs) on cubic zinc oxide (c‐ZnO) is reported, which is used as an inorganic electron transport layer in optoelectronic devices, via a facile spin‐coating method. The PeSCAs consist of rectangular thin microplatelets of 6–10 µm in length and 2–3 µm in width. The deposited c‐ZnO enables the formation of phase‐pure and highly crystallized cubic perovskites via an epitaxial lattice coherence of (100)CsPbBr3∥(100)c‐ZnO, which is further confirmed by grazing incidence wide‐angle X‐ray scattering. The PeSCAs demonstrate a significant structural stability of 26 days with a 9 days excellent photoluminescence stability in ambient environment, which is much superior to the perovskite nanocrystals (PeNCs). The high crystallinity of the PeSCAs allows for a lower density of trap states, longer carrier lifetimes, and narrower energetic disorder for excitons, which leads to a faster diffusion rate than PeNCs. These results unravel the possibility of creating the interface toward c‐ZnO heterogeneous layer, which is a major step for the realization of a better integration of perovskites and charge carrier transport layers.
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