Highly ordered three-dimensional nanostructure thin films provide substantially increased surface area for organic attachment and new detection principles due to the new and unique optical and physical properties of the nanostructures. Upon organic material attachment, the optical birefringence of these highly ordered three-dimensional nanostructure thin films changes due to screening of polarization charges. The surfaces of the highly ordered three-dimensional nanostructure thin films are thus suitable candidates for studying organic adsorption for sensing and chromatography applications. We review contemporary research in this area and specifically report the monitoring of organic attachment using the generalized ellipsometry and quartz crystal microbalance with dissipation techniques. Both methods are sensitive to the adsorption of organic layers, on the order of few angstroms to few micrometers in thickness, at the solid-liquid interface. The combinatorial use of both techniques, described in Chap. 11, provides insight toward how organic materials attach within highly ordered three-dimensional nanostructure thin films. We discuss studies of fibronectin protein adsorption, decanethiol chemisorption, and cetyltrimethylammonium bromide adsorption. We also address potential future developments and applications.