Actinide peroxide nanospheres and uranyl selenate nanotubules represent the first examples of nanoscale structures in actinide compounds. Very frequently, formation of nanostructures corresponds to organic-inorganic composites with clearly defined interfacial interactions. This chapter describes the character of these interactions with the use of charge-density matching concept with some modifications related to the basic chemical properties of actinides. Most of the reported nanostructured actinide compounds are obtained under soft synthesis conditions. Most of these compounds are soluble and it is rather hard to foresee any practical application of them. However, findings demonstrate the possibility of nanoscale fabrication for actinides in higher oxidation states. A whole new range of uranium-based nanotubular and nanocomposite materials can be synthesized. One possible application of these materials is the utilization of depleted uranium, hundreds of thousands of tons of which are now stored by nuclear countries.