Structure control over soft matter on a molecular through nanoscopic lengthscale is a vital tool to optimizing properties for applications ranging from energy (solar and thermal) to biomaterials. For example, while molecular structure affects the electronic properties of semiconducting polymers, the crystal and grain structure greatly affect bulk conductivity, and nanometer lengthscale pattern of internal interfaces is vital to charge separation and recombination in photovoltaic and light emission effects. Similarly, biological materials gain functionality from structures ranging from monomeric sequence through chain shape through self-assembly. We work to both understand the effects of structure on properties and gain pattern control in these inherently multidimensional problems.