In this study, polyindole (PIN)/TiO2 nanocomposites were synthesized with and without the presence of sodium dodecylsulfate, anionic surfactant, with two different PIN contents. The synthesized materials were subjected to various characterizations namely: particle size, apparent density, conductivity, dielectric constants, magnetic susceptibility, elemental analysis, Fourier transform infrared spectroscopy spectroscopy, thermogravimetric analysis, X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. Characterization results revealed the successful preparations of PIN/TiO2 hybrid nanocomposites. Electrokinetic properties of all the materials were determined by zeta (zeta)-potential measurements in aqueous and nonqueous media. Effects of pH, temperature, presence of various electrolytes, and surfactants on electrokinetic properties of the materials were examined.