T he tunability of chemical synthesis and material fabrication enables polymeric biomaterials to display diverse chemical and mechanical properties. Recent strides in decoupling methodologies, especially surface-patterning and combinatorial techniques, offer much promise in further understanding the structure-function relationships that largely govern the success of future advancements in biomaterials, tissue engineering, and drug delivery. This follows with examples of more effective decoupling techniques, mainly from the perspective of three primary classes of synthetic materials: polyesters, polyethylene glycol, and polyacrylamide. Relevant examples of coupled material properties are briefly reviewed in each section to highlight the need for improved decoupling methods. In this article, we discuss three basic decoupling strategies: (1) surface modification, (2) cross-linking, and (3) combinatorial approaches (i.e., copolymerization and polymer blending). Structure-function relationships can be more clearly understood by the effective decoupling of each individual parameter. However, due to the coupled nature of material properties, their individual effects on cellular responses are difficult to understand. Therefore, a fundamental understanding of how individual material properties modulate cell-biomaterial interactions is pivotal to improving the efficacy and safety of clinically translatable biomaterial systems. Determining how a biomaterial interacts with cells (“structure-function relationship”) reflects its eventual clinical applicability.
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