Macromolecular materials that are capable of selectively and efficiently localizing cells, factors, and/or drugs offer important approaches for mediating biological events and in the development of hybrid materials. We have employed a combination of biosynthetic tools, bioconjugation strategies, and biomimetic assembly to produce thermoresponsive (poly)peptides derived from sequences of resilin, elastin, and collagen. These materials can be designed to control localization of biomolecules with tunable microscale mechanics, and materials with select properties have demonstrated promise for healing vascular graft materials in vivo. In addition, these types of materials not only show controllable micro- and nanoscale morphologies, but also have promise for targeted drug delivery to damaged tissue in vivo.