Nanofluids which consist of the addition of nanoparticles in a base fluid are envisaged for a large domain of applications. For many of them, the surface tension (ST) behavior of the prepared nanofluids is a key parameter to exploit their thermophysical properties. Due to their remarkable properties, carbon nanotubes (CNTs) are commonly used to develop nanofluids. However, the evolution of the ST of CNT-based nanofluids is still far from being understood and predictable. In the present work, two base fluids were used: water and a commercial mixture of propylene-glycol/water (around 40:60 wt%). The impact of the used multi-walled CNT (MWCNT) addition, MWCNT concentration (0.001 and 0.1 wt%) and temperature variation (273.15–333.15 K) on the density and ST evolution for the two kinds of CNT-based nanofluids is studied. The chemically modified MWCNTs are assumed to bear both localized hydrophilic areas due to grafted functional groups and remaining hydrophobic surfaces. The found difference in ST behavior between the two types of nanofluids is explained in light with the involved interfaces in each nanofluid. ST evolution is found to strongly depend on the CNT surface properties.