[EN] A new method to significantly enhance the photoelectrochemical properties of phenyl-modified carbon nitride layers via the insertion of nickel ions into carbon nitride layers is reported. The nickel ions: are embedded within the carbon nitride layers by manipulating the interaction of Ni ions and molten organic molecules at elevated temperature prior to their condensation. A detailed analysis of the chemical and photophysical properties suggests that the nickel ions dissolve in the molten molecules, leading to the homogeneous distribution of nickel atoms within the carbon nitride layers. We found that the nickel atoms can alter the growth mechanism of carbon nitride layers, resulting in extended light absorption, charge transfer properties, and the total photoelectrochemical performance. For the most photoactive electrode, the Ni ions have an oxidation state of 2.8, as confirmed by soft X-ray absorption spectroscopy. Furthermore, important parameters such as absorption coefficient, exciton lifetime, and diffusion length were studied in depth, providing substantial progress in our understanding of the photoelectrochemical properties of carbon nitride films. This work opens new opportunities for the growth of carbon nitride layers and similar materials on different surfaces and provides important progress in our understanding of the photophysical and photoelectrochemical properties of carbon nitride layers toward their implantation in photoelectronic and other devices. We thank the use Katz Institute for Nanoscale Science & Technology Ben Gurion University for HR-TEM measurements. M.S. thanks Dr. Laurent Chabanne for fruitful discussion. K.M.L. is grateful for the support by the Helmholtz Association (VH-NG-1140). Zhang, W.; Albero-Sancho, J.; Xi, L.; Lange, KM.; García Gómez, H.; Wang, X.; Shalom, M. (2017). One-Pot Synthesis of nickel-modified carbon nitride layers toward efficient photoelectrochemical cells. ACS Applied Materials & Interfaces. 9(38):32667-32677. https://doi.org/10.1021/acsami.7b08022