The effect of the zeta potential of nano zero-valent iron (nZVI) and carbocatalyst on the activation of persulfate was investigated. The oxidation experiments were performed on three different compounds, with variously modified nZVI and three distinct carbocatalysts. From the obtained results, an evident linear correlation between nanoparticles’ zeta potential and reaction rate constants of these three compounds oxidation may be observed. This phenomenon is not mechanism-specific and occurs for the radical and non-radical processes. The present work indicates the critical influence of the surface charge of nZVI and carbocatalysts on the persulfate catalytic activation.