Atomically precise, noble metal nanoclusters (NCs) smaller than ~2 nm in diameter are an emerging area of nanoscience. NCs are currently of intense fundamental interest for their unique electronic properties, and have considerable practical appeal due to their potential use in nanoparticle-based devices that require precise control of structure at the atomic level. Their novel optical properties, in particular, make them attractive as components for high resolution displays, sensing, and photo-controlled drug delivery. We have been exploring routes to systematically control composition and morphology of well-defined, mono-disperse copper NCs and superatoms. We are particularly interested in studying copper because it an earth abundant first row metal, and copper nanoparticles have been shown to be active towards CO₂ reduction and other catalytic transformations. These results will guide the methodology needed for the rational syntheses of nanomaterials using elements from across the periodic table. The use of a variety of spectroscopic techniques, including X-ray diffraction, neutron diffraction, and XAS, in conjunction with kinetic and reactivity studies, yield unique insights into the structure-function relationships present in nanomaterials.