In the past decade, the synthesis, characterization and application of nanomaterials has become a major research area in the chemical and biological sciences with numerous research centers and institutions dedicated to this field. While many synthetic chemists and materials scientists have produced countless novel nanomaterials, the full characterization of the products is far less developed. We have been studying the fundamental chemistries both structural and dynamic at the interface of nanomaterials with NMR spectroscopy. A combination of solution- and solid-state NMR methods is implemented to elucidate the capping chemistry and organization of biomolecular ligands at the surface of nanomaterials. The primary goal of this work is to develop “easy to implement” NMR techniques to provide standard structural characterization for functionalized nanoparticles and nanomaterials.