Hollow carbon sphere–implanted graphitic carbon nitride nanosheet photocatalysts were prepared by a bottom-up method. The photocatalysts promote photoelectron transfer and suppress charge recombination through special interface coupling and hollow carbon spheres as an electron acceptor, leading to remarkably improved photocatalytic efficiency. This work thus provides an efficient pathway for the design of efficient and low-cost cocatalysts for photocatalysis. More information can be found in the Full Paper by D. Jing, J. Tang et al. (DOI: 10.1002/chem.202102330).