Al-doped carbon nanotubes(Al-doped CNTs) were prepared as a multifunctional integrated material of adsorbent and coagulant aid for organic pollutant removal from aqueous solution. It was observed that aluminum species were dispersed homogeneously on the surface of CNTs, and mainly anchored onto defect structures of the CNTs. The introduction of aluminium efficiently improved adsorption ability for methyl orange(MO) onto the CNTs,and maximum adsorption capacity calculated from the Langmuir isotherm model can reach 69.7 mg/g. The MO adsorption kinetics can be better described by the pseudo-second-order and pore diffusion kinetic models, and the diffusion of MO anions into pores of the Al-doped CNT adsorbent should be the rate-determining step.Thermodynamic analyses indicated that the adsorption of MO onto Al-CNTs-2.0 was endothermic and spontaneous. Moreover, adsorption capacity for MO on the Al-doped CNTs was evidently dependent on the CNT dose, solution p H and adsorbent dose. From the perspective of low-cost and multifunctional, suspension obtained during the Al-doped CNT adsorbent preparation, was tested as coagulant to remove humic acid(HA). A significant observation is that the suspension exhibited an excellent coagulation performance for HA,because abundant aluminous polymer and Al-doped CNTs existed in the suspension. Al-doped carbon nanotubes (Al-doped CNTs) were prepared as a multifunctional integrated material of adsorbent and coagulant aid for organic pollutant removal from aqueous solution. It was observed that the aluminum species were dispersed homogeneously on the surface of CNTs, and mainly anchored onto The structures of the CNTs. The introduction of aluminum efficiently improved adsorption ability for methyl orange (MO) onto the CNTs, and maximum adsorption capacity calculated from the Langmuir isotherm model can reach 69.7 mg / g. the pseudo-second-order and pore diffusion kinetic models, and the diffusion of MO anions into pores of the Al-doped CNT adsorbent should be the rate-determining step. Thermodynamic analyzes indicated that the adsorption of MO onto Al-CNTs-2.0 was endothermic and spontaneous. Moreover, adsorption capacity for MO on the Al-doped CNTs was evidently dependent on the CNT dose, solution p H and the adsorbent dose. From the perspective of low-cost and multifunctional, suspension obtained during the Al-doped CNT adsorbent preparation, was tested as coagulant to remove humic acid (HA). A significant observation is that the suspension exhibits an excellent coagulation performance for HA, because of an abundant aluminous polymer and Al-doped CNTs existed in the suspension.