The aim of this study was to characterize and compare the zeta potential of particles sensitive to external thermal stimuli. Poly N-(isopropyl) acrylamide (PNIPA) was selected as the thermosensitive polymer with a volume phase transition temperature (VPTT) between 32 and 33 °C. The hydrodynamic diameter (D) of the nanoparticles was measured by dynamic light scattering. Zeta potential (ZP) measurements were performed with the same instrument used for D measurements. ZP measurements allow the prediction of the stability of colloidal systems in aqueous solutions. These measurements were combined with a pH study before and after the purification process of the particles. The ZP was measured to determine the electrostatic interactions between the particles, which can lead to particle aggregation and decrease their colloidal stability. The effect of the composition of the synthesized particles on the ZP was assessed. One of the most important factors influencing ZP is pH, especially in aqueous solutions. The initiator did not significantly affect the D of the particles, but it did significantly affect the ZP. The synthesized particles were subjected to a visible radiation absorption study in the selected temperature range to determine the VPTT.