The research focuses on the innovative use of graphite‐like carbon nitride (gC3N4) catalysts along with supercritical carbon dioxide (scCO2) for the green synthesis of valuable organic compounds. Having explored different synthetic routes for gC3N4 and the obtained samples efficiency in the photocatalytic oxidation of benzyl alcohol with molecular oxygen in scCO2, we identified the most effective catalyst bearing ether linkers between layers of a graphite‐like structure. This catalyst facilitates the production of benzaldehyde and benzoic acid derivatives, highlighting the potential for sustainable industrial applications. The study's emphasis on a metal‐free catalyst and a zero‐waste process underlines its contribution to environmentally friendly chemical practices. The proposed approach offers a more sustainable and efficient alternative to traditional processes in small‐scale chemical production.