A hybrid composite based on metal-organic framework (MOF) was chemically fabricated by embedding the magnetic Fe3O4 nanoparticles within amino-functionalized porous La-MOF (MOF/NH2) to produce a highly efficient and reusable composite of MOF/NH2/Fe3O4. Different proper techniques were used for the characterization of surface morphology and chemical arrangement of the prepared MOF/NH2/Fe3O4 composite. The characterization results using various techniques including Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscope (SEM), Brunauer, Emmett, and Teller analysis (BET), and vibrating sample magnetometer (VSM) approved the successful fabrication of MOF with amino arms on its surface besides the well magnetization using magnetic nanoparticles. The MOF/NH2/Fe3O4 composite showed enhanced adsorption capacity (618 mg/g) toward methyl orange (MO) anionic dye which is higher than many commercial reported adsorbents due to the presence of many types of adsorption sites (NH2 groups and lanthanum sites), large surface area of MOF, and the synergetic effect of magnetic nanoparticles. Moreover, the MOF/NH2/Fe3O4 composite showed selective adsorption of MO dye from dye mixtures owing to the electrostatic attraction. Also, the MOF/NH2/Fe3O4 composite retained over 90% of its efficiency for the dye removal even after six successive cycles. So, the present study provided a practical strategy for the design of functional MOF hybrid composites. Furthermore, due to the adaptability of its architectural form, it is a potential adsorbent material for industrial wastewater treatment uses.