A primary interest in the Wooley laboratory is the production of functional polymers from renewable sources that are capable of reverting to those natural products once their purpose has been served. The inherent stereochemical and functional diversities of natural products provide opportunities to expand the scopes and complexities of polymer materials, by utilizing fundamental synthetic organic chemistry approaches. This presentation will highlight synthetic strategies for the development of polymers, block polymers and crosslinked network materials, which can be produced by relatively simple approaches from complex polyhydroxyl natural products and can be made to exhibit a range of properties. It is expected that the physical, mechanical, supramolecular assembly and stability properties will be tuned by the chemical compositions and structures, controlled by the advancement of synthetic methodologies by which to prepare such materials. Polycarbonates and polyphosphoesters that can be produced rapidly as well-defined block polymers and then undergo multiple chemical transformations and direct assembly in water into functional nanomaterials are serving as platforms for several directions toward their development as biomedical devices for the treatment of lung infections and osteosarcoma lung metastases. If time allows, recent developments toward the preparation of functional polypeptides and their assemblies will also be described.