Polycyclic aromatic hydrocarbons and their derivative nanostructures serve as the fundamental organic inventory of the universe. Far from static, these species undergo a complex evolutionary pathway transitioning from isolated gas-phase molecules to hybrid three-dimensional architectures, such as hydrogenated amorphous carbon and fullerenes. This mini-review reflects recent breakthroughs across observational, laboratory, and theoretical astrochemistry. With the advent of the James Webb Space Telescope, we can now resolve the fine spatial and spectral structures of photodissociation regions and distant star-forming galaxies (z ~ 1–2), tracking specific topological defects in carbon skeletons. Parallel to these observational milestones, laboratory action spectroscopy utilizing cryogenic ion traps has definitively linked the C₆₀⁺ cation to diffuse interstellar bands and revealed ultrafast radiative cooling mechanisms via recurrent fluorescence. On the theoretical front, we highlight the critical shift from harmonic models to anharmonic cascade emission and the deployment of ab initio metadynamics to simulate fullerene assembly. Finally, we explore how machine learning and neural network potentials are breaking computational bottlenecks, enabling on-the-fly kinetic modeling of amorphous dust growth.