Nanoparticles have aroused widespread interest because of their unique surface structure and nano effect, which presents novel characteristics like as sound, light, electricity, magnetism, and thermal properties. However, two critical defects have hindered their applications: (1) poor processability resulting from the high melting temperature (e.g., >1000 °C) for some inorganic nanoparticles; (2) the restriction of the nano effect caused by the easy aggregation of the nanoparticles. To solve those issues, solvent-free nanofluids (SNFs) with hard cores and flexible organic chains were successfully designed and fabricated at the beginning of the twenty-first century. The promising technology of SNFs not only solved the dispersion problem of nanomaterials but also imparted novel functionalization to nanoparticles. Up to now, many researchers have been devoted to developing diverse cores and flexible organic polymer chains to endow SNFs with particular functions, such as conductivity, fluorescence, lubricity, and so on. However, there are few review reports on the research progress in the fabrication and applications of functional SNFs. To gain a better understanding of SNFs, this paper presents an overall investigation into the development, fabrication, as well as the applications of functional SNFs.