Carbon nitride polymers have emerged as a new class of materials for a wide range of applications such as photo- and electro-catalysis, sensors, bioimaging and more due to their chemical, photophysical and catalytic properties as well as their low-price, facile synthesis and high stability under harsh chemical conditions. In this review we begin with a broad overview of carbon-based materials, arriving at the focus of this review, polymeric carbon nitrides (CNs). After a brief overview of applications, we delve into their various synthetic methods, with an emphasis on achieving control on the nanoscale features of this intriguing polymeric semiconductor. The main synthetic pathways include co-polymerization at various stages, templating, an ionothermal pathway and harnessing of supramolecular pre-organization, which are discussed in detail along with CN growth and deposition on substrates. Finally, we give our perspectives on the evolution of this field, the current limitations, and elaboration of achievable control over the chemical composition, the electronic structure and the morphology of this family of materials.