The strategic objective of the carbon nanostructures activity is to control the synthesis and functionality of nanocarbon building blocks e.g. fullerenes, nanotubes, nanohorns, graphene. To achieve this aim, the design of their surface/interface properties using different synthesis, top-down as well as bottom-up approaches and doping processes is of paramount importance. In order to fully exploit the outstanding properties of those synthetic carbon allotropes, chemical functionalization is required and modification of their framework plays a key-role. Covalent and non-covalent chemical transformations considerably improve and tailor the solubility and processability of carbon nanostructures and at the same time combine their properties with those of the added chemical moieties. We are interested and explore the fundamental properties of carbon-based nanostructured materials. We have introduced a plethora of diverse organic molecules (porphyrins, phthalocyanines, corroles, pyrenes, perylenes, phenylenevinylenes, aminoacids, peptides) as well as nanoparticles (i.e. quantum dots, carbon dots) onto fullerenes, carbon nanotubes/nanohorns and graphene. By employing our wet-chemistry knowledge, we synthesize new nanocarbon-based architectures performing in electron donor-acceptor schemes for managing photo-induced electron-transfer processes and targeting mainly energy conversion applications. We employ an arsenal of spectroscopic techniques to characterize the newly derived hybrid carbon-based nanomaterials and we explore their physicochemical, photophysical and electrochemical properties. We also apply advanced electrochemical tools to assess the electrocatalytic performance of the developed carbon-based nano-architectures toward energy-related key electrochemical reactions (hydrogen production, oxygen evolution, oxygen reduction) as well as electro-oxidation of small organic molecules.