Large‐Scale Synthesis of Monodispersed Perovskite Nanocrystals via Autonomous Continuous Droplet Microfluidics

ABSTRACT The scalable synthesis of perovskite nanocrystals (PNCs) with monodispersity and high emission efficiency remains a significant challenge, primarily limited by the inherent constraints of flask‐based batch synthesis in handling large volumes. Here, we propose a novel microscale continuous droplet‐in‐flow synthesis (µ‐CDFS) of PNCs stabilized by zwitterionic ligands. This synergy, arising from the spatial and temporal separation of droplet‐based reactors and a cross‐locked PNC‐ligand surface coordination, ensures exceptional mixing efficiency and consistency. Consequently, our approach enables the scalable production of high‐quality PNCs, delivering a continuous output of 0.8 g h − 1 per channel, a narrow size distribution (σ r < 14%), and a photoluminescence quantum yield (PLQY) exceeding 97%. Furthermore, high‐throughput ligand screening is also performed via autonomous flow experimentation, and the emission of PNCs is precisely tuned across the visible region (453–753 nm) via on‐demand halide anion exchange, establishing a robust platform for the accelerated discovery of PNCs.