Solution-processed colloidal quantum dots (CQDs) are a promising class of semiconducting materials in view of their tunable optical and electronic properties through the quantum size effect. [1][2][3][4][5] They have been used to fabricate nextgeneration thin-film optoelectronic devices including light-emitting diodes, [6] photodetectors, [7] and solar cells. [8][9][10][11][12][13] For example, recent perovskite quantum dotbased light-emitting devices showed an external quantum efficiency exceeding 20%. [14][15][16][17] Solar cells based on lead chalcogenide CQDs have demonstrated power conversion efficiencies (PCE) of 11.3% [18] and a stabilized output over 150 days when stored in air even without encapsulation, [19] making them candidates for low-cost, stable, and scalable next-generation photovoltaics.While the performance of CQD solar cells has improved rapidly, the fabrication process is still limited to labscale, batch-processing methods, mainly due to reliance on a complex and wasteful multistep layer-by-layer (LbL) ligand exchange method, [20] which to date has been most commonly combined with repeated spin-casting deposition. To overcome this limitation, a solution-phase ligand exchange method was recently developed to realize the single-step fabrication of CQD films. [21][22][23] In particular, inorganic anions such as metal chalcogenide complexes, halides, and metal-free ions (S 2− , OH − , SCN − , etc.) have been successfully applied as capping ligands and improved the colloidal dispersion. However, CQDs capped with anions-CQD inks-are typically dispersed in highboiling-point solvents such as N, N-dimethylformamide (DMF) or N-methylformamide (MFA), which adds complexity to the production of sufficiently thick CQD films. [24] To produce CQD films directly from CQD inks, various approaches have been demonstrated, including centrifugal casting [7] and supersonic spray coating. [25] However, so far, these methods have been limited in scale to batch-processing; large-scale, single-step QD film formation has not yet been realized.One of the main challenges when forming films from CQD inks is to inhibit (or even control) the spatial redistribution of the dispersed solute during late-state evaporation. [26] This redistribution often results in poorly controlled film morphology Solution-processed colloidal quantum dots (CQDs) are attractive materials for the realization of low-cost and efficient optoelectronic devices. Although impressive CQD-solar-cell performance has been achieved, the fabrication of CQD films is still limited to laboratory-scale small areas because of the complicated deposition of CQD inks. Large-area, uniform deposition of lead sulfide (PbS) CQD inks is successfully realized for photovoltaic device applications by engineering the solute redistribution of CQD droplets. It is shown experimentally and theoretically that the solute-redistribution dynamics of CQD droplets are highly dependent on the movement of the contact line and on the evaporation kinetics of the solvent. By lowering the f...