Transfer of the excellent intrinsic properties of individual carbon nanoparticles into real-life applications of the corresponding heat transfer fluids remains challenging. This process requires identification and quantification of the nanoparticle-liquid interface. Here, for the first time, we have determined geometry and properties of this interface by applying transmission electron cryomicroscopy (cryo-TEM). We have systematically investigated how the particle morphology of carbon-based nanomaterials affected the thermal conductivity, specific isobaric heat capacity, thermal diffusivity, density, and viscosity of ionanofluids and/or bucky gels, using a wide range of fillers, especially single-walled carbon nanotubes (SWCNTs) and multi-walled carbon nanotubes (MWCNTs) – both with extreme values of aspect ratio (length to diameter ratio) from 150 to 11,000. Accordingly, hybrid systems composed of various carbon nanomaterials and ionic liquid, namely 1-ethyl-3-methylimidazolium thiocyanate [EMIM][SCN], were prepared and characterized. Most of the analyzed nanodispersions exhibited long-term stability even without any surfactant. Our study revealed that the thermal conductivity could be remarkably improved to the maximum values of 43.9% and 67.8% for ionanofluid and bucky gel (at 1 wt% loadings of MWCNTs and SWCNTs), respectively, compared to the pristine ionic liquid. As a result, the model proposed by Murshed and co-workers has been improved for realistic description of the concentration-dependent thermal conductivity of such hybrid systems. The obtained results undoubtedly indicate the potential of ionanofluids and bucky gels for energy management.