NanoFullerenes is an ambitious interdisciplinary project to understand the top-down formation process of fullerene molecular nanostructures in space, involving the destruction/processing of hydrogenated amorphous carbon (HAC) nanoparticles and similar natural materials like asphaltenes and kerogen. By understanding this, NanoFullerenes will allow us to unveil another significant open questions in astrochemistry. The detection of fullerenes in the H-rich circumstellar environments of evolved stars and diverse astrophysical environments show that formation of these complex species does not require a H-poor environment contrary to general expectation. The identification of the fullerene cation C60+ as a diffuse interstellar band (DIB) carrier (the only DIB carrier known to date) together with recent progress on cosmic fullerenes reinforce the idea that these molecular nanostructures are ubiquitous in space. NanoFullerenes goes beyond the state-of-the-art by combining organic chemistry synthesis, top-level lab experiments, novel machine-learning approaches for quantum-chemistry calculations, and unprecedented astronomical data. The proposed project has strong potential to challenge our current understanding of the chemistry of large organic molecules as well as the chemical processing in space