Our group’s research centers on molecular-scale materials design to address pressing challenges in sustainable chemistry, with a primary focus in catalytic and adsorption applications. Synthetic methods to prepare these materials largely involve tuning coarse-grained parameters (e.g., concentration, temperature), often resulting in structures with poorly controlled distributions of molecular architectures. Since these architectures dictate the physicochemical and optoelectronic properties that govern performance in a given application, controlling them is paramount. To achieve this control, our work takes a molecular-scale approach to materials synthesis. By manipulating molecular precursors and their interactions early in the synthetic process (i.e., prior to nucleation), we can introduce new control parameters that influence the assembly of building units across length scales, and address a key bottleneck – the synthesis-structure component – in the iterative synthesis-structure-function elucidation process that guides rational materials design.