Dynamic functionality in living systems is regulated by catalysis and self-assembly, and especially the interplay between them. It also provides a powerful approach for the introduction of dynamic aspects in materials science and nanotechnology, giving access to dynamic properties were both kinetics of formation and properties and spatial locale of the structures formed may be regulated. In doing so, we are developing understanding of how function arises from molecular organization, complexity and dynamics. Specifically, the approach enables incorporation of dynamic response mechanisms into materials- essentially synthetic metabolism. We are investigating a number of applications of biocatalytic self-assembly, including controlling motility, controlling supramolecular order in electronic materials, and the use of self-assembly peptides to control the catalytic/oxidative formation of synthetic melanin-like materials, etc.