Developing resilient soft materials optimized for load-bearing and toughness is a long-standing challenge which, if solved, could enable the design of advanced resins, fabrics, packages, separation technologies, and tissue replacements. Inspired by the graded and hierarchical s tructures of natural marine materials, this IRG aims to (i) develop new strategies for materials processing that integrate precise, discrete polymer chemistries with non-equilibrium processing methods to achieve controlled multi•phase and interfacial structure, (ii) understand the interactions and mechanics of internal interfaces in these materials, and (iii) establish the multiscale structure-property relationships to provide the foundational design rules for creating new classes of versatile, multi phase soft materials.