In this paper, we present a study on thermal conductivity and viscosity of nanofluids containing novel atomic layer deposition surface-modified carbon nanosphere (ALD-CNS) and carbon nanopowder (ALD-CNP) core-shell nanocomposites. The nanocomposites were produced by atomic layer deposition of amorphous TiO2. The nanostructures were characterised by scanning (SEM) and transmission electron microscopy (TEM), energy dispersive X-ray analysis (EDX), Fourier transform infrared spectroscopy (FT-IR), Raman spectroscopy, thermogravimetry/differential thermal analysis (TG/DTA) and X-ray powder diffraction (XRD). High-concentration, stable nanofluids were prepared with 1.5, 1.0 and 0.5 vol% nanoparticle content. The thermal conductivity and viscosity of the nanofluids were measured, and their stability was evaluated with Zeta potential measurements. The ALD-CNS enhanced the thermal conductivity of the 1:5 ethanol:water mixture by 4.6% with a 1.5 vol% concentration, and the viscosity increased by 37.5%. The ALD-CNS increased the thermal conductivity of ethylene–glycol by 10.8, whereas the viscosity increased by 15.9%. The use of a surfactant was unnecessary due to the ALD-deposited TiO2 layer.