In this Perspective, we discuss a novel water-splitting scenario, namely the direct oxidation of water molecules by organic photooxidants in hydrogen-bonded chromophore-water complexes. In comparison with the established scenario of semiconductor-based water splitting, the distance of electron transfer processes is thereby reduced from mesoscopic scales to the Ångström scale, and the time scale is reduced from milliseconds to femtoseconds, which suppresses competing loss processes. The concept is illustrated by computational studies for the heptazine-H2O complex. The excited-state landscape of this complex has been characterized with ab initio electronic-structure methods and the proton-coupled electron-transfer dynamics has been explored with nonadiabatic dynamics simulations. A unique feature of the heptazine chromophore is the existence of a low-lying and exceptionally long-lived 1ππ* state in which a substantial part of the photon energy can be stored for hundreds of nanoseconds and is available for the oxidation of water molecules. The calculations reveal that the absorption spectra and the photochemical functionalities of heptazine chromophores can be systematically tailored by chemical substitution. The options of harvesting hydrogen and the problems posed by the high reactivity of OH radicals are discussed.