This Account details key developments in dimensional control of contorted aromatics for organic electronics. Coronene, perylene, pyrene, and [4]helicene, which are fragments of graphene, can be contorted using facile synthetic chemistry into large nanoribbons and nano‐architectures. In comparing contorted or higher‐dimensional graphene architectures to planar or lower‐dimensional species, the materials properties are reliably enhanced for the contorted aromatics. Examples of enhanced properties include optical absorptivity, conductivity, device photoconversion efficiency, and solubility. These enhancements are exemplified in organic photovoltaics, photodetectors, field effect transistors, and perovskite solar cells. Described herein are key advances in dimensional control of contorted aromatics that have resulted in world record photoconversion efficiencies, photodetection capabilities matching inorganic state‐of‐the‐art devices, and ∼5 nm long ultrathin soluble graphene nanoribbons.