An efficient organic/inorganic magnetic nanohybrid of MgAl@CuFe2O4-polylysine was successfully synthesized and employed as a suitable adsorbent for removal Cr(VI) and methyl orange from water solution. The prepared nanohybrid was characterized by X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, vibrating sample magnetometer and thermogravimetric analysis. The nanohybrid of MgAl@CuFe2O4-polylysine was employed to adsorb anionic species, i.e., Cr(VI) and methyl orange through electrostatic attraction, ligand exchange and ion exchange. Multivariate optimization with Box-Behnken design was used to evaluate effective parameters such as dosage of adsorbent, solution pH and contact time on adsorption and their interaction. Results showed that pH, contact time and adsorbent dosage are effective parameters for Cr(VI) adsorption; however, the pH of the solution is the sole effective parameter for methyl orange adsorption. Both analyte adsorptions are fast with adsorption times less than 15min. Isotherm study revealed that the prepared nanohybrid is a highly efficient adsorbent for methyl orange and Cr(VI) with adsorption capacity of 693.6 and 281.8mg g-1, respectively. Isotherm study showed that adsorption of both analytes well fitted with the Freundlich adsorption isotherm model, which indicated multilayer adsorption on the heterogeneous surface. The magnetic saturation for the prepared adsorbent was 12.64 emu g-1, which was adequate and suitable for magnetic separation of samples. The prepared adsorbent was regenerated using ethanol-aquaeous NaOH solution as it shows 90% removal efficiency after three cycles.