Synthetic photochemistry is a research field, where organic transformations are promoted by the presence of photoactive species, under light irradiation. In particular, the sub‐field of photo‐organocatalysis, where organic molecules are used as photocatalysts, has been launched as a “green” and sustainable approach. Carbon allotrope nanostructures (CANs) and their derivatives exhibit unique photophysical and photochemical properties, which have been exploited for the preparation of efficient metal‐free and sustainable photocatalytic systems. This review summarizes the progress on the field of photochemical carbocatalysis, presenting the achievements by fullerene‐, carbon nanotube‐ and graphene‐based nanomaterials. Additionally, future prospects for CAN‐based nanomaterials as photochemical promoters for organic transformations are also mentioned.