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Nowadays, nanoscience is strongly intertwined with the biological and medical fields. The functional effectiveness of nanomaterials depends not only on their chemical composition but also on their structural and surface features. In this respect, shape, size, and atomic surface terminations play a key role. One of the most important and challenging parameters of customization of metal and metal oxide nanoparticles is the shape control that can provide the desired optical, electrical, and magnetic properties. The chemical tuning of the morphology following the known synthetic strategies can be exploited in the biomedical application, specifically imaging techniques such as MRI and SERS to build a nano-amplifier and provide higher contrast and clarity in the resulting images. Further, when speaking of biomaterials, other relevant properties come into the spotlight: besides the relevance of the morphological features, atomic features of the surface structure have an effect on the destiny of the interaction of these materials with a host biological system. Hence, understanding the biomaterial surface characteristics at the fundamental level can improve the control in designing the new materials that could be more effective in the applied field. This aspect is considered, particularly on hydroxyapatite-and silica-based nano-biomaterials. Furthermore, the relevant properties of the luminescent lanthanide-containing hydroxyapatite nano-biomaterials, of high importance in the bioimaging field, are also highlighted. On the whole, this chapter discusses the structural engineering and surface features of inorganic materials including metallic and ceramic ones.