The surface of three different kinds of coal was modified by three surfactants (cationic, anionic, and non-ionic). Changes on coal surface were examined by the zeta potential technique. The influence of the dispersion of pH, concentration of surfactants, and contact time were investigated. The most significant change in zeta potential resulting from adding surfactants was observed in activated coal (hydrophobic surface, largest BET surface area). Adding the cationic surfactant led to an increase of the zeta potential, contrary to measuring done in water. The anionic surfactant decreased the value of the zeta potential; however, this change was not too remarkable. The results proved that even a very low concentration of the cationic surfactant (0.01 mmol/L) causes a remarkable change of the zeta potential. On the other hand, a similar effect was observed until the concentration of the anionic surfactant reached about 10 mmol/L. The mechanism of binding surfactants is not simple, but preferential hydrophobic interactions were discovered.