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 cm2 min−1 from 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.