In this paper, the structural and zeta potential properties of 10-hydroxycamptothecin (HCPT) were investigated by FT-IR and zeta potential analyzer under different pH. The anticancer drug HCPT as a model drug was used to prepare a high-performance and relatively easy-to-fabricate system on Fe3O4 magnetite nanoparticles by using a polystyrene sulfonate (PSS) and HCPT interlayer self-assembly method. The results obtained from FT-IR and XRD confirmed that HCPT was molecularly dispersed into the nanoparticles. The method holds not only environment-friendly characteristics and the ability to mimic the self-organization process in biological systems but also greatly decreases adjuvant polymers. In addition, the system has an ideal drug payload for the delivery of insoluble HCPTs.