This dissertation explores the structure, chemical reactivities, electromagnetic response, and materials properties of various carbon nanostructures, including single-walled carbon nanotubes (SWCNTs), multi-walled carbon nanotubes (MWCNTs), graphite, and graphene nanoribbons (GNRs). Efficient production and modification of these unique structures, each with their own distinct properties, will make them more accessible for applications in electronics, materials, and biology. A method is reported for controlling the permittivity from 1–1000 MHz of SWCNT-polymer composites (0.5 wt%) for radio frequency applications including passive RF antenna structures and EMI shielding. The magnitude of the real permittivity varied between 20 and 3.3, decreasing as higher fractions of functionalized-SWCNTs were added. The microwave absorbing properties and subsequent heating of carbon nanotubes were used to rapidly cure ceramic composites. With less than 1 wt% carbon nanotube additives and 30–40 W of directed microwave power (2.45 GHz), bulk composite samples reached temperatures above 500°C within 1 min. Graphite oxide (GO) polymer nanocomposites were developed at 1, 5, and 10 wt% for the purpose of evaluating the flammability reduction and materials properties of the resulting systems. Microscale oxygen consumption calorimetry revealed that addition of GO reduced the total heat release in all systems, and GO-polycarbonate composites demonstrated very fast self-extinguishing times in vertical open flame tests. A simple solution-based oxidative process using potassium permanganate in sulfuric acid was developed for producing nearly 100% yield of graphene nanoribbons (GNRs) by lengthwise cutting and unraveling of MWCNT sidewalls. Subsequent chemical reduction of the GNRs resulted in restoration of electrical conductivity. The GNR synthetic conditions were investigated in further depth, and an improved method which utilized a two-acid reaction medium was found to produce GNRs with fewer defects and/or holes on the basal plane and higher aspect ratio. Two different covalent functionalization methods for GNRs based on diazonium chemistry were developed. The resulting functionalized GNRs (f-GNRs) are readily soluble in organic solvents which increase their solution processability. The f-GNRs were also found to be in a reduced state, with minimal sp2 carbon disruption, while also keeping the ribbon shape.