The adsorption of Cr(VI) and Ni(II) using ethylenediaminetetraacetic acidmodified diatomite waste (EDTA-DW) as an adsorbent in single and binary systems was investigated. The EDTA-DW was characterized using various analytical techniques, including Fourier transform infrared spectroscopy, thermogravimetric analysis, Brunauer-Emmett-Teller measurements, X-ray diffraction, scanning electron microscopy and energy-dispersive spectrometry.The adsorption experiment was conducted by varying pH, adsorbent dosage, initial concentration and temperature. In the single system, the sorption data for Cr(VI) fitted the Langmuir isotherm, but the Ni(II) adsorption data fitted well the Freundlich isotherm. The maximum sorption capacity of Cr(VI) and Ni(II) was 2.9 mg g −1 at pH = 3 and 3.64 mg g −1 at pH = 8, respectively. The kinetic data for both Cr(VI) and Ni(II) followed well the pseudo-second-order kinetic model in single and binary systems. Meanwhile, the extended Langmuir and extended Freundlich multicomponent isotherm models were found to fit the competitive adsorption data for Cr(VI) and Ni(II). In addition, in the binary system, the existence of Ni(II) hindered the adsorption of Cr(VI), but the presence of Cr(VI) enhanced the removal of Ni(II). This study provides some realistic and valid data about the usage of modified diatomite waste for the removal of metal ions.