Optimizing Printed Quasi‐2D Luminescent Perovskite Films via Delaminated Metal–Organic Framework Modulation

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Microelectronic printing technology has recently emerged as a key approach in advancing pixel‐array perovskite films, particularly quasi‐2D perovskite films, to meet current scientific and technological demands. However, its further development remains hindered by the uncontrollable crystallization of perovskite during the printing process. Herein, a novel in situ heterogeneous nucleation growth approach for obtaining quasi‐2D perovskite films is demonstrated, utilizing delaminated metal–organic frameworks (i.e., layered Cd‐MOF) with an ordered structure as modulators. The inosculation of phenylethylammonium (PEA + ) with layered Cd‐MOF serves as crystal nuclei, facilitating heterogeneous crystal nucleation and growth while regulating the distribution of the n‐phase. Moreover, the intercalation of the layered Cd‐MOF alleviates rigid stress, thereby eliminating defects in the printed films. The resulting quasi‐2D perovskite films exhibit an impressive photoluminescence quantum yield of 37.40% along with exceptional luminescent stability, making them promising candidates for various optoelectronic applications. Overall, this study highlights the significant potential of MOF‐assisted synthesis in advancing high‐performance perovskite materials through microelectronic printing technology, offering a promising pathway for the development of future optoelectronic devices.