Molecular biorecognition is at the heart of all biological processes and has come to the center stage in designing new biologics. Coiled-coils result from molecular biorecognition of multiple protein α-helices. We have designed a series of coiled-coil motifs that self-assemble into supercoils, which in turn function as physical cross-linkers in the construction of hybrid biomaterials. This dissertation describes our endeavors following the hypothesis below: the selfassembly of coiled-coil

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... g peptides into coiled-coils can be used as a cross-linking mechanism in the construction of hybrid hydrogels and the development of a drug-free macromolecular therapeutic. In the first part, a macromonomer free radical copolymerization strategy was developed and HPMA graft copolymers containing coiled-coil motifs of different chain lengths were synthesized. Results indicated that the primary structure of these motifs greatly influenced gel formation. At least four heptads were needed to mediate effective gelation. The gelation process was highly dependent on the environmental temperature and copolymer concentration. In the second part, a drug-free macromolecular therapeutic was designed to take full advantage of the facts that CD20 is one of the most reliable biomarkers for B-cell non-Hodgkin's lymphoma (NHL), and cross-linking of CD20 antigens induces apoptosis of B cells. The drug-free therapeutic was composed of two components: Fab' fragment of 1F5