Exotic graphene nanocarbon allotropes are composed of pure graphene sheets morphed into unusual shapes. These structures exhibit the exceptional properties of graphene, including high strength, superior electrical and thermal conductivity, electromagnetic field (EMF) shielding, catalytic activity, unique transport and semiconductor characteristics, and lightweight behavior. The exotic morphologies of these nanocarbon allotropes can focus and further tailor graphene’s properties. For example, coiled and complex three-dimensional structures can significantly influence a material’s torsional spring strength, EMF shielding capacity, and catalytic efficiency. This chapter presents the synthesis, spectroscopy, and analysis of exotic graphene nanocarbon allotropes. It details the high-purity preparation of structures such as nano-bamboo, nano-pearl, and spiral graphene nanoallotrope, as well as helical and nano-tree carbon nanotube morphologies. These graphene-based nanostructures are produced via a unique decarbonization chemistry known as C2CNT® (CO2 to Carbon Nanotechnology). This method is designed to mitigate the existential threat of climate carbon by carbon capture and transforming CO2 through transition metal-nucleated electrolytic splitting. By tailoring the electrochemical parameters—including temperature, current density, and the composition of the anode, cathode, and electrolyte—the process converts CO2 into various graphene nanocarbons (GNCs) and oxygen. The reaction occurs in molten carbonates by passing current from an anode to a cathode, following the general reaction: CO2 → GNC + O2.