Nature has long been a source of fascination, inspiration and humility for chemists. Despite our best efforts, the rate enhancements delivered by our catalysts fall orders of magnitude short of those achieved by enzymes, our drug delivery systems do not offer the selectivity and efficiency of viruses, and our materials do not have the ability to self-organize, self-repair and adapt to our changing needs the way that biological supramolecular polymers, such as the cytoskeleton does. A common theme in the above examples is nature's use of proteins to achieve these goals. Based on this premise, we set out to devise a method for hierarchically programming the self-assembly of a monomeric protein into functional materials. By using metal ions as the "molecular glue" that holds these complexes together, we have overcome many of the traditional issues in programming their assembly and shown that an unprecedented degree of chemical and thermal stability can be imparted on the protein subunits. Although we have not yet achieved the level of sophistication demonstrated by natural systems, our approach, which combines the fields of coordination chemistry, supramolecular chemistry, and computational design, has allowed us to assemble a single molecular precursor into a range of potentially useful structures