The need to mimic the structures and functions of proteins with synthetic constructs arises with increasing frequency in research and technologies related to drug delivery, new biomaterials and other molecular, cellular and tissue therapeutics. Most of the fundamental issues in these areas are interfacial in nature. Molecules must be deployed effectively at interfaces to manipulate interactions. Self-assembly is a potentially useful route to accomplish this. Molecular structure at interfaces is crucial to controlling functions. In this talk, examples from our group and other will be discussed to lay out the state-of-the-art in mimicking protein function with synthetic constructs.