This article describes the preparation of a nanoadsorbent containing Co-nanoparticles decorated functionalized SiO2-Al2O3 mixed-oxides as a scavenger toward removal of methyl orange. SiO2-Al2O3 mixed-oxides were functionalized with pyridine-2-carbaldehyde and thereafter, in the next step, Conanoparticle was prepared over the modified mixed-oxides. The as-prepared nanoadsorbent was characterized by Fourier transform infrared (FTIR), UV-visible diffuse reflectance spectra (UV-vis DRS), inductively coupled plasma atomic emission spectroscopy (ICP-AES), Brunauer-Emmett-Teller (BET), transmission electron niicroscopy (TEM), electron paramagnetic resonance (EPR), cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). Results showed that Co-nanoparticle with average size of about 5-25 nm was immobilized successfully on the surface of modified mixed-oxides and was widely dispersed. EPR and CV of Si/Al-PAEA = PyCA@CoNP confirmed that most of the covalently bond active sites of the nano-adsorbent are in the form of Co(II) ions. The supported cobalt is a suitable and efficient adsorbent for the removal of methyl orange from aqueous solution. The heterogeneous Co-NPs were found to be effective adsorbent for the removal of methyl orange ions from solution. The adsorption process was spontaneous and endothermic in nature and followed pseudo-second-order kinetic model. The CV and EIS of the Co-NP5-MO indicates an easily oxidizable environment, this being in agreement with the FTIR data, where the electron density at Co-NPs is higher due to the presence of a donor-electron ligand (methyl orange), that is, reduction of Co-NPs from +3 to +2 oxidation state is more favored. (C) 2014 Elsevier Inc. All rights reserved.