The control over the chemical and electronic properties of carbon nitride‐based materials is highly challenging due to limitations of the traditionally used solid‐state reaction. Tailoring parameters, such as morphology, surface area, or energy band positions, in this kind of materials is essential for the improvement of the overall performance in a given application, namely photo‐ or electrocatalysis, sensing, or water treatment, amongst others. The supramolecular preorganization of carbon‐nitrogen based monomers via non‐covalent interactions prior to the thermal condensation has made it possible to design graphitic carbon nitride‐like (CN) materials and target specific properties. In this review, we discuss the latest developments in the synthesis of CN and other carbon‐based materials from the supramolecular preorganization of monomers and the consequences on the photocatalytic performance. The monomer sequence, solvent, and reaction conditions which determine the final structure of the supramolecular assembly, and therefore the final CN properties after calcination, are thoroughly discussed.