In this study, the enhancement of ZnO’s dielectric properties is pursued through the manipulation of its particle size using a surfactant-based approach. The synthesis of ZnO nanoparticles with the aid of surfactants is achieved through the sol–gel method. Through x-ray diffraction analysis, the formation of the desired Wurtzite structure is confirmed, with no secondary phases detected. The surface characteristics of the synthesized powders are examined through scanning electron microscopy (SEM) and transmission electron microscopy (TEM), both of which highlight the even distribution of the surfactant-assisted nanoparticles. The crystallite size is quantified using Scherrer’s formula. UV-visible spectroscopy and photoluminescence are employed to delve into the optical properties. Dielectric behavior is assessed across a frequency range of 20 Hz to 4000 kHz at room temperature. Comparative analysis between ZnO samples grown with and without surfactants reveals that those with surfactant assistance display heightened capacitance, a notably higher dielectric constant, increased AC conductivity, and longer transit time.