Understanding and manipulating transformations of CO2, O2, H2O, NO3–, CH4, and N2 is crucial for establishing sustainable energy cycles, and using inputs such as electricity or light allows coupling of these reactions to renewable sources. Developing platforms that can activate these molecules is a continuous challenge and must be approached from many directions. As such, we take inspiration from homogeneous molecular, heterogeneous materials, and biological enzyme catalysis to create more effective platforms. This dissertation describes this general approach and then focuses on a supramolecular strategy that integrates the structural tunability of molecular porphyrin catalysts into a rigid and porous architecture that benefits from a materials-inspired high surface area. This platform is widely applicable, showing various improvements in the catalysis of CO2, O2, and H2O reduction. We also present a bio-molecular platform that combines a synthetic porphyrin catalyst with bio-inspired additives that can function as electron and proton mediators resulting in improved CO2 reduction. Overall, our general strategy for blurring the lines between molecular, materials, and biological fields of catalysis has proven fruitful and aids in the rational design of more optimized systems.