The application of covalently attached ferrocene groups to the aluminum-silicate nanoparticles (ASNPs) for phosphate (P) removal from the synthetic and real waters has been studied and the prepared nanomaterials were analyzed by XPS, EDS, BET, TEM, chemical analysis (CHN), FTIR, and ICP-AES. The immobilization of the ferrocene on the surface of the inorganic support (mixed oxides) can lead to reduce the drawback of the pristine ferrocene molecules which may have strong tendency to agglomerate into larger particles, resulting in the negative effect on both available active sites and catalyst performance. XPS of Fe ions evidenced that most of the active sites of the nano-adsorbent is in the form of Fe(III) ions at the surface. The heterogeneous Fe(III) ions were effective toward removal of phosphate. The contact time to obtain equilibrium for maximum adsorption of phosphate (100%) was found to be 120 min. The adsorption kinetics of P has been evaluated in terms of pseudo-first- and -second-order kinetics, and the Freundlich and Langmuir isotherm models have also been tested to the equilibrium adsorption results. The adsorption process was spontaneous and endothermic in nature and followed pseudo-second-order kinetic model. FTIR, EDS and XPS results confirmed the formation of Fe-O-P bond on the Si/Al@Fe surface after adsorption of P from aqueous media. The Si/Al@Fe displayed high reusability due to its high removal capacity after 10th adsorption-desorption runs. The proposed adsorbent could also be utilized to adsorb the P ions from the real sample (Persian Gulf water). The high removal capacity of P ions from the real water and the high levels of reusability confirmed the versatility of the heterogenized ferrocene groups on the ASNPs. (C) 2015 Elsevier Inc. All rights reserved.