A series of Fe3O4@mesoporous-silica-pillared clays (Fe3O4@MSPCs) with different pore size are synthesized using cationic polymeric surfactant templating. These materials possess uniform pore size and the magnetic nanoparticles generated onto the intergallery silica pillar. The polymeric surfactant (PVA-1488) plays a key role to tune both the pore size of the materials and the particle size of Fe3O4. These materials show better performance of lysozyme loading and releasing, as a potential slow-releasing delivery for macromolecule drugs.