From the most classic carbon materials (CMs) to the advanced ones, all of them integrate a promising catalyst set in terms of sustainability and energy efficiency for a greener future. Different synthetic strategies concerning to the catalytic synthesis of relevant N‐containing heterocycles are herein described to address the great potential of the referred catalysts flying over what has been done and all that remains to be done. Current trends in this field involve structure‐activity relationships establishment also considering the reaction mechanisms understanding and the identification of active catalytic sites, as function of both experimental datasets, emphasizing on operando characterization techniques, and theoretical studies which will significantly contribute to the design of custom‐made catalysts as a new horizon. Building N‐heterocycles by using CMs. Current trends for the sustainable synthesis of significant N‐containing heterocycles, considering both different synthetic approaches to construct the heterocyclic core, and the role of CMs used as catalysts and catalyst supports, are reviewed. Establishment of structure‐activity relationships and reaction mechanisms understanding can contribute, in the future, to the rational catalyst design as a new horizon.