The ability of natural and modified clay to adsorb phenol was studied. The clay samples were analyzed by different technical instruments, such as X-ray fluorescence (XRF), X-ray diffraction (XRD) and FT-IR spectroscopy. Surface area, pore volume and average pore diameter were also determined using B.E.T method. Up to 73 and 99% of phenol was successfully adsorbed by natural and activated clay, respectively, from the aqueous solution. The experiments carried out show that the time required to reach the equilibrium of phenol adsorption on all the samples is very close to 60 min. The amount of phenol adsorbed shows a declining trend with higher pH as well as with lower pH, with most extreme elimination of phenol at pH 4. The adsorption of phenol increases proportionally with the initial phenol concentration. The maximum adsorption capacity at 25 °C and pH 4 was 29.661 mg/g for modified clay (NaMt). However, the effect of temperature on phenol adsorption was not significant. The simple modification causes the formation of smaller pores in the solid particles, resulting in a higher surface area of NaMt. The equilibrium results in aqueous systems were well fitted by the Freundlich isotherm equation (R2 > 0.98). Kinetic studies showed that the adsorption process is best described by the pseudo-second-order kinetics (R2 > 0.99). The adsorption of phenol on natural and modified clay was spontaneous and exothermal.