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i) Photo showing the separation between acetonitrile (ACN, on the top) and methylamine (MA)-containing ethanol (EtOH, on the bottom) in the ink at the initial state. ii) Scheme showing the initial state of ACN-EtOH binary ink system containing pristine and E1-coated perovskite intermediate dissolved in different solvent medium. iii) Scheme showing the formation of E1-perovskite intermediate cluster (PIC) micro-emulsion phase in the ink upon solvent mixing. iv) Scheme showing the migration of E1-PIC emulsion phase toward top part of wet film during solvent evaporation. v) The final bilayer film consisting of top layer crystallized from E1-PIC micro-emulsion phase and bottom layer crystalized from pristine larger perovskite intermediate clusters.

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