Biological materials serve as a continual source of inspiration for the design and development of new materials due to their unique combination of properties. These properties are often the result of the hierarchical arrangement of organic and inorganic components that are formed through multiple assembly mechanisms. My research focuses on designing materials and processing methods that can leverage a combination of self-assembly and non-equilibrium processing to create hierarchically structured materials. As an example of this work, I will present my research on the self-assembly of poly(ethylene oxide-propylene oxide-b-ethylene oxide) block copolymers (BCPs) in epoxy consisting of a bisphenol A diglycidyl ether (BADGE) monomer and an ionic liquid latent curing agent for use as a 3D-printable thermoset or as a high-toughness adhesive. My research is aimed at addressing three critical knowledge gaps that have previously dampened attempts to design these materials: 1) understanding the influence of the ionic liquids on the self-assembly of the block copolymers, 2) identifying key chemical mechanisms for the ionic liquid-induced epoxy crosslinking, and 3) linking the impact of processing to the evolution of the structure and properties of the materials. Addressing these knowledge gaps has been possible through a combination of rheology, small angle x-ray scattering, microscopy, thermal analysis, and spectroscopy. While I have made significant progress in understanding these critical structure-property-processing relationships, the potential variable space is infinite and our traditional Edisonian experimental approaches are insufficient to be able to design materials on demand. To conclude this talk, I will turn an eye to the future and describe my efforts to utilize high throughput experimentation and machine learning to accelerate our ability to navigate through the complex variable space and enable the co-design of the materials and processes. These approaches enable us to develop a deeper understanding of the structure-property-processing relationships towards the development of epoxy/block copolymer blends for use as multifunctional nanocomposites and high toughness coatings and adhesives.