In this study, the adsorption behavior of phenol onto natural sediments from Liaohe River was studied. The effect of pH, temperature, ionic strength, and surfactants on the adsorption process was also investigated. Results showed that it took 48 h for the phenol to achieve adsorption equilibrium on sediment. Kinetic analysis indicated that the process fit well with the intraparticle diffusion model. The phenol adsorption process was pH dependent with the maximum adsorption at pH 4.58. With respect to the Freundlich and Langmuir models, the DR isotherm can describe the adsorption process better. Thermodynamic parameters revealed that phenol adsorption was physisorption. The coexistent salt and surfactants at relatively higher concentrations inhibited the phenol adsorption on Liaohe River sediment.