A surfactant-modified coal fly ash was developed as a multifunctional adsorbent for the removal of organic pollutants from wastewater. Sodium dodecyl sulfate (SDS) was used to modify the surface of coal fly ash (CFA). The modified CFA was characterized using scanning electron microscopy (SEM), surface porosity analyzer, thermogravimetric analysis (TGA) and Fourier transform infrared (FTIR) spectroscopy. The results showed that loading CFA with SDS not only improved the functionality and surface morphology of the raw ash for the adsorption of organic pollutants, but also enhanced its thermal stability. The efficiency of the modified fly ash was tested in terms of removal of two non-polar organic pollutants namely chlorobenzene (CB) and nitrobenzene (NB) from aqueous phase. The maximum uptake capacity of chlorobenzene and nitrobenzene with SDS-modified coal fly ash (SCFA) was 225 mg/g and 90 mg/g, respectively. The kinetic analysis was done by controlled kinetic models, i.e., pseudo first and second order kinetic models. The results showed that adsorption of CB and NB onto SCFA followed a pseudo second order kinetic model. The adsorption of chlorobenzene was exothermic over the modified adsorbent while nitrobenzene showed an endothermic behavior. The isotherm analysis depicted the multilayer adsorption of both pollutants onto the surface of the surfactant modified adsorbent. This work has shown that surface modification using surfactants can be a viable option to enhance the adsorption capacity of fly ash for pollutants removal.