A further aim of this study was to demonstrate the utility of Sc-based photoredox catalysis. We chose arenecarbonitriles, which serve as crucial structural scaffolds in synthesising bioactive compounds, alongside their substantial role as intermediates in organic synthesis. We particularly focused on the direct photooxidative cyanation of the aromatic C-H bond, as this reaction remains a formidable challenge for the chemical community because of the need for prefunctionalised starting material and the lack of regioselectivity.