Both tissue engineering and biological science will benefit from a generalized methodology to create multilayered cellular architectures that mimic tissue structures found in vivo. Elastin-like polypeptides (ELPs) are tandemly-repeated polymers derived from a portion of the primary sequence of mammalian elastin. ELPs have previously been used for protein purification, nucleic acid delivery, and thermally-mediated targeting of solid tumors. The ELP was produced in E. coli and purified by the inverse temperature transition purification method. The ELP was conjugated with several polyelectrolytes using carbodiimide activation chemistry. These conjugates were characterized by FTIR spectroscopy, XPS, mass spectroscopy, and the ninhydrin assay. These conjugates were used as scaffold materials for primary rat hepatocytes and H35 rat hepatoma cells. Hepatocyte-specific urea and albumin production were quantified under a variety of culture conditions. These approaches may represent a promising class of biomaterials for a variety of tissue engineering applications.