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Nanocomposites based on hyperbranched polymers (HBPs) and layered silicates as nanofillers are a relatively new class of nanocomposites. Due to their unique physical/chemical properties, they have attracted scientific interests. This book provides to a better understand the structure-dynamics-properties relationship, for different types of HBP/ kaolinite (Ka) nanocomposites via a combination of different methods. The molecular dynamics was studied by means of broadband dielectric spectroscopy (BDS). The dielectric spectra are dominated by the conductivity contribution at higher temperatures, for all samples investigated. The segmental dynamics ( -relaxation) revealed by specific heat spectroscopy (SHS). In the framework of this book, it was evident that the method of the preparation of the nanostructures, the end-groups of HBPs, the concentration of the nanofiller, and the treatment of its surface have a significant effect on preparing exfoliated or intercalated nanocomposites. Thus, new nanocomposites with tailor-made properties could be obtained. To sum up, at the moment, it looks like that there is still no limit and no end for studies on HBPs nanocomposites.