The bottom-up synthesis of graphene nanomaterials has recently emerged as an important approach for accessing carbon materials featuring desirable or exotic electronic properties. The ability to produce these materials with structural precision and synthetic flexibility makes bottom-up synthesis a powerful tool both for understanding materials at the nanoscale and for designing the next generation of high-performance nanomaterials. Although a handful of robust bottom-up synthetic techniques has been developed, investigation has been quite limited with regard to both the types of graphene nanomaterials produced and the applications for which those materials are considered. In this thesis, the extant tools of bottom-up synthesis are applied to the production of novel zero-dimensional and one-dimensional graphene nanomaterials. This includes the use of surface-assisted techniques for the synthesis of unique nanographenes featuring exotic electronic and magnetic properties, facilitated by development of a robust and general solution chemistry methodology to access challenging acene derivatives. This work also examines the unprecedented application of bottom-up synthesized one-dimensional graphene nanoribbons (GNRs) as composite materials with inorganic nanoparticles, and describes the exceptional performance these diverse composites achieve through the rational design of nanomaterial interfaces.