AbstractThe synthesis of a set of new organic photocatalysts (PCs) with a donor-acceptor carbazolyl dicyanobenzene structure is reported. The PCs developed have fine-tailored redox potentials from –1.62 V (PC•+/PC*) to 1.36 V (PC*/PC•–) and were accessed through a straightforward two-step synthesis. The potential of these PCs was demonstrated in synthetically relevant reactions with mechanistically opposite thermodynamic requirements, previously reported only in the presence of precious Ir-based PCs. In addition, the PCs outperformed the yields promoted by the well-established 4CzIPN organic dye in both type of reactions.