The design of organic molecules is not only an academic curiosity for scientists but has also contributed significantly to the evolution of science and technology. Nonplanar π-systems with distinct three-dimensional shapes, such as bowls, waves, hoops, helices, and spheres, represent an important class of molecules due to their beautiful structures and characteristic functions. To promote the use of such essential molecules in materials science, procedures for their synthesis need to be scalable. Fullerenes, corannulenes, helicenes, calix[n]arenes, cycloparaphenylenes, and pillar[n]arenes meet this standard, and have found diverse applications in organic electronics, optical materials, supramolecular assemblies, and molecular recognition (Figure ). This wide range of applications highlights the potential of readily available nonplanar π-systems to facilitate the creation of next-generation materials. However, the current syntheses of nonplanar π-systems heavily rely on the stepwise formation of bonds between their constituent fragments, which is known as the 'bottom-up' approach. The limited number of synthetic pathways to create nonplanar π-systems inevitably results in impractical molecular frameworks.