Adsorption is an effective method for treating wastewater containing nickel due to its minimal equipment requirements and flexible operation. Therefore, an environmental friendly, inexpensive, efficient and recyclable adsorbent is needed. In this work, a reusable dual-functional super-paramagnetic adsorbent was prepared by combining APTES (3-Aminopropyltriethoxysilane) and EDTA (ethylenediaminetetraacetic acid disodium) with magnetic diatomite for the removal of Ni2+. It is named diatomite/CoFe2O4@APTES-EDTA (DECFASEs). The synthetic material was characterized and studied by XRD (X-ray Powder Diffractometer), FTIR (Fourier Transform Infrared Spectrometer), SEM (Scanning Electron Microscope), TEM (Transmission Electron Microscope), EDS (Energy Dispersive Spectrometer), VSM (Vibrating-Sample Magnetometer), BET (Brunauer-Emmett-Teller) method, Zeta potential analyzer and XPS (X-ray Photoelectron Spectroscopy), respectively. The performance of adsorption Ni2+ by DECFASEs was studied on effect of pH, reaction time and initial concentrations. The adsorption and desorption capacity and recyclability of the adsorbent material were estimated. A adsorption kinetic data had a significant correlation with the pseudo second-order kinetic and also adsorption isotherm data corresponded well with Freundlich adsorption isotherm. The maximum adsorption capacity of the adsorbent material was 19.22 mg/g. The Ni2+ adsorption capacity of DECFASEs decreased slightly from 9.11 to 8.25 mg/g after 4 recycles. The XPS results of DECFASEs before and after Ni2+ uptake showed N and O participated in the complexation of Ni2+ in the adsorption process, which verified the chemical interaction between Ni2+ and DECFASEs. Modified-diatomite is a promising adsorbent for aqueous Ni2+ removal.