transistors, [1] displays, [2] solar cells, [3] and biosensors. [4] In particular, meniscus-guided coating (MGC) such as zone casting, [5] slot die coating, [6] and solution shearing [7] is especially promising due to their compatibility to industrially relevant "sheet2sheet" and "roll2roll" processes. [8] For solution shearing, solution is sandwiched between a heated substrate and a blade, [9] where the solution forms a curved air-liquid interface (i.e., meniscus); as the blade moves, thinfilm is generated across the substrate due to solidification (i.e., a process involving supersaturation of the solution, followed by nucleation and growth) occurring near the meniscus. [10] Here, the thin-film properties (e.g., crystal alignment, crystal size) are strongly dependent on the solidification process, which in turn determines the performance of the thin-film device. Therefore, it is of critical significance to understand how the experimental parameters affect the solidification process so that it can be precisely controlled.The determining factors that affect solidification process are the fluid dynamic phenomena occurring near the meniscus, [10,11] such as capillary flow, Marangoni flow, viscous drag, and solvent evaporation. [12] Each of these effects is intricately dependent on multiple solution shearing parameters (e.g., shearing speed, substrate temperature), is complexly intertwined to affect theThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.202105035.