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Solution-processed thin-film perovskite solar cells (PSCs), where the record efficiency has rocketed from 3.8% to 22.1% — comparable to commercial silicon-based solar cells — in just seven years, offer unprecedented promise of low-cost, high-efficiency renewable electricity generation. Hybrid organic-inorganic perovskites(HOIPs) at the heart of PSCs have unique structures, which entail rotating organic cations inside inorganic cages, imparting them with desirable optical and electronic properties. To exploit these properties for PSCs application, the reliable deposition of high-quality HOIP thin films over large areas is critically important. The microstructures and grain-boundary networks in the resulting polycrystalline HOIP thin films are equally important as they control the PSC performance and stability.Fundamental phenomena pertaining to synthesis, crystallization, coarsening, and microstructural evolution involved in the solution-based- and amine-gas-based-processing of HOIP thin films for PSCs will be discussed with specific examples. The overall goal of our research is to have deterministic control over scalable processing of tailored HOIP thin films with desired compositions, microstructures, and grain-boundary networks for large-area, high-efficiency, and stable PSCs.