Inorganic catalysts have been workhorses in many important industrial processes while many biological systems, such as photosynthesis, rely on organic catalysts. In this talk I will discuss the use of computational chemistry to examine organic catalysts and photocatalysts for visible light activated atom transfer radical polymerization (ATRP) and CO2 reduction into fuels. In both cases, dearomatization of the catalysts leads to powerful reducing agents capable of challenging reductions either by electron transfers or hydride transfers. Using various substituents the thermodynamic and kinetic properties of these catalysts can be optimized for various reductions to make them fast, yet energy efficient. Our ATRP photocatalyst designs were synthesized and characterized for their efficacy, which confirmed that the best designs effectively photocatalyze polymerizations by ATRP using visible light and result in polymers and block copolymers with no metal contamination and properties that rival the best materials catalyzed with optimized, but expensive metal catalysts.