Gold nanorods have potential applications as chemical sensing, biological imaging, and photothermal therapeutics. Our laboratory has developed the syntheses of these materials, in controlled size and shape, over the last few years. Surface modification of these nanomaterials is a key step to enable applications. In this talk I will describe our recent efforts to wrap up nanorods with layer-by-layer polyelectrolyte deposition in aqueous solution, in a way that allows for “capture coating” of small molecules at defined distances from the surface; how we can “fix” the surface of the nanomaterials by on-particle polymerization reactions; and how surface ligand exchange and overcoating affects biological properties of these materials.