Synthesis, design, characterization, and application of carbon-based nanostructures (CBNSs) as drug carriers have attracted a great deal of interest over the past half of the century because of their promising chemical, thermal, physical, optical, mechanical, and electrical properties and their structural diversity. CBNSs are well-known in drug delivery applications due to their unique features such as easy cellular uptake, high drug loading ability, and thermal ablation. CBNSs, including carbon nanotubes, fullerenes, nanodiamond, graphene, and carbon quantum dots have been quite broadly examined for drug delivery systems. This review not only summarizes the most recent studies on developing carbon-based nanostructures for drug delivery (e.g. delivery carrier, cancer therapy and bioimaging), but also tries to deal with the challenges and opportunities resulting from the expansion in use of these materials in the realm of drug delivery. This class of nanomaterials requires advanced techniques for synthesis and surface modifications, yet a lot of critical questions such as their toxicity, biodistribution, pharmacokinetics, and fate of CBNSs in biological systems must be answered.