Montmorillonite (MMT) based anisotropic magnetic nanoparticles (Fe3O4/APTES/MMT) with high anisotropy and reliable magnetism were prepared by using Fe3O4 as magnetic nanoparticles and gamma-aminopro pyltriethoxysilane (ATPES) as modifier. The characterization indicated that the interactions between Fe3O4 nanoparticles and MMT in Fe3O4/APTES/MMT were stronger than that of directly deposited on to MMT (Fe3O4-MMT) because APTES was chemically bonded to both Fe3O4 and MMT. Fe3O4/APTES/MMT had a greater Ms value (25.16 emu/g) than Fe3O4-MMT (23.71 emu/g). Also, ultrasonication was used to test the interactions between Fe3O4 and MMT. With 30 min of ultrasonication, the amount of Fe3O4 nanoparticles on the surface of Fe3O4/APTES/MMT was more than that of Fe3O4-MMT, and Fe3O4/APTES/MMT had a faster magnetic response to a magnetic field than that of Fe3O4-MMT because of enhanced interactions between Fe3O4 and MMT in Fe3O4/APTES/MMT. In addition, Fe3O4 nanoparticles were densely immobilized onto Fe3O4/APTES/MMT with a smaller average diameter, and the distribution of Fe3O4 nanoparticles on the surface of MMT was more uniform than that of Fe3O4-MMT. Fe3O4/APTES/MMT possessed stable and high magnetism, in ease of orientation and recycling in the magnetic field, and this makes it a promising candidate as anisotropic nanoparticles for use in preparing anisotropic inorganic/polymer composites and anisotropic adsorbents used in wastewater treatment. Finally, the mechanism of ATPES-modified magnetic MMT was investigated. (C) 2018 Elsevier B.V. All rights reserved.