Magnetic magnesium ferrite (MgFe2O4) nanoparticles (MMFNPs) were synthesized by employing the sol-gel method. These nanoparticles were ultrasonically decorated onto the multi-walled carbon nanotubes (MWCNTs) to produce magnetic magnesium ferrite nanocomposites (MMFNCs). The as-prepared materials were investigated for their capability to treat wastewater loaded with heavy metals. The synthesized nanocomposites were characterized by field emission scanning electron microscopy, transmission electron microscopy, X-ray diffraction, Fourier transmission infrared spectroscopy, Raman spectroscopy, thermogravimetric analysis, and zeta analyzer. Besides, the effect of the environmental chemistry of the solution was determined by varying the critical parameters. The adsorption isotherm of Cr(VI) adsorption onto the as-synthesized MMFNC best fitted the Langmuir adsorption isotherm model. The high adsorption capacity of 175.43 mg/g was achieved at a temperature of 40 °C under optimized conditions. Due to the magnetic nature of MMFNC, they are easily recoverable from the aqueous solution making them cost-friendly. Even after seven consecutive adsorption-desorption cycles, the MMFNC presented an efficiency loss of less than 20% for the removal of Cr(VI) ions. The presented development method offers prospects in developing a highly effective magnetic adsorbent for heavy metal removal from wastewater.