Nanostructured particles (NSPs), with their remarkable properties at the nanoscale, possess key functions required for unlocking a sustainable future. Fabricating these particles using aerosol methods and spraying processes enables precise control over the particle morphology, structure, composition, and crystallinity during in-flight transformation. In this Perspective, the significant impact of NSPs on technological advancement for energy and environmental applications is discussed. Furthermore, incorporating in situ/operando assessment techniques alongside machine and deep learning is explored. Finally, the future development trends and the perspective on the advancing NSPs synthesis via aerosol process are elaborated for further driving innovations for supersmart and carbon-neutral society.