 Graphitic carbon nitride, GC3N4, has emerged as an attractive metal-free visible light photocatalyst due to its advantages of earth abundance, nontoxicity, and stability. However, its photocatalytic efficiency is seriously limited by charge carrier's ready recombination and their low reaction dynamics. Modifying the local electronic structure of GC2N4 is predicted to be an efficient way to improve the charge transfer and reaction efficiency. This article was authored by Junwei Fu, Kang Lu, Kersen Jiang, and others.