Magnetic materials are fundamental to technologies today and the future. Although usually associated with bulk metals, single molecular magnets based on transition metals have shown promise in emerging fields such as nanoelectronics. Recently, fundamental studies have uncovered the magnetic properties of carbon-based materials, i.e. with open shell structure or unpaired pi-electron dubbed as pi-radicals. However, such studies are usually either in a purely theoretical point of view or under ultra-high vacuum conditions and cryogenic temperatures. These are the main limits to realizing new magnetic carbon-based materials. Thus, this project (Synthesis of π-Magnetic Molecular Materials, SpiM) aims to: to contribute new π-magnetic molecules realizable in bulk by solution-phase methods; and (2) to explore their incorporation into functional molecular architectures and devices. Successful achievement of the objectives will introduce novel magnetic materials for future technologies. Such carbon-based materials could be critical in the shift from of organic materials from their inorganic materials, which may face environmental, socio-political, and economic problems related to their mining.