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An extremely rapid process for self‐assembling well‐ordered, nano, and microparticle monolayers via a novel aerosolized method is presented. The novel technique can reach monolayer self‐assembly rates as high as 268 cm²min⁻¹from a single aerosolizing source and methods to reach faster monolayer self‐assembly rates are outlined. A new physical mechanism describing the self‐assembly process is presented and new insights enabling high‐efficiency nanoparticle monolayer self‐assembly are developed. In addition, well‐ordered monolayer arrays from particles of various sizes, surface functionality, and materials are fabricated. This new technique enables a 93× increase in monolayer self‐assembly rates compared to the current state of the art and has the potential to provide an extremely low‐cost option for submicron nanomanufacturing.

Smart windows are energy‐efficient windows whose optical transparency can be switched between highly transparent and opaque states in response to incident solar illumination. Transparent and conductive metal nanomesh (NM) films are promising candidates for thermochromic smart windows due to their excellent thermal conductivity, high optical transparency at near infrared wavelengths, and outstanding stability. In this study, ZnO/Au/Al₂O₃NM films with periodicities of 200 and 370 nm are reported. The ZnO/Au/Al₂O₃NM film with a 370 nm periodicity exhibits a transmittance over 90% at 550 nm and sheet resistance lower than 20 Ω sq⁻¹. Based on a standard figure of merit, this structure outperforms current state‐of‐the‐art NM films. Here, the integration of ZnO/Au/Al₂O₃NM films into a thermochromic perovskite smart window is also demonstrated. The transparency of the smart window structure is manipulated by transient resistive heating to trigger the thermochromic transition to the opaque state, which can be then maintained solely by 1‐sun, AM 1.5 G illumination. This climate‐adaptive, low power‐activated, and fast‐switching smart window structure opens new pathways toward its practical application in the real world.