Attapulgite-zeolite composite nano-structure adsorbent was manufactured using natural attapulgite and zeolite. The obtained adsorbent was characterized by scanning electron microscope, energy dispersive X-ray spectrometer and mercury porosimeter. After elementary characterization of this adsorbent, batch tests were carried out to examine its removal mechanism of phenol. The influence of pH, contact time and initial phenol concentration were investigated. The pH variation studies showed that the optimum pH for adsorption of phenol was found to be 7. Adsorption equilibrium attained within 1 h time. The adsorption process followed pseudo-second-order kinetic model. Adsorption isotherm studies showed that Langmuir model fitted the experimental data better than Freundlich model. The attapulgite-zeolite composite nano-structure adsorbent in this study shows very good promise for practical applicability of phenol removal from aqueous solution.