Antonietti and coworkers on its photocatalytic properties in 2009. [1] Originally a niche subject of academic curiosity from the works of Berzelius, Liebig, [2] and Gmelin [3] nearly 200 years ago, interests in this material family was first revived as a proposed precursor to the computationally postulated ultrahard ß-C 3 N 4 in the 1990s. [4] In the last decade, the surge in publications on g-C 3 N 4 materials arose primarily due to their favorable photo-/electro-chemical properties, especially for the photocatalytic synthesis of solar fuels such as hydrogen from water-splitting, a research direction motivated by concerns over the environmental and socio-political impacts of our reliance on fossil fuels. Many of these publications focus on the catalytic aspects of this class of materials, aiming to improve their reaction kinetics through chemical modification or material processing. In