In this work, the harvesting of Nannochloropsis oculata microalgae through the use of nanosized Fe3O4 immobilized in polyvinyl alcohol (PVA)/sodium alginate (SA) as a flocculant (Fe3O4/PS) is investigated. Using the Fe3O4/PS immobilized beads could reduce the amount of soluble ferrous ions (Fe2+) released from naked Fe3O4 in acid treatment, leading to easy recovery. The characterization was performed under different dosages and pH values of Fe3O4/PS. The results show that the Fe3O4/PS, when applied to the algae culture (500 mg dry cell weight/L), achieves a 96% harvesting efficiency under conditions of a pH of 4 with 200 mT magnetic field intensity. Fe3O4/PS can be directly reused without adjusting the pH value. The recycled Fe3O4/PS shows stability in terms of its surface properties, maintaining more than 80% harvesting efficiency after five recycles. Magnetophoretic harvesting, using immobilized magnetic iron oxide as a particle-based flocculant, is a potential method to reduce challenges related to the cost-effective microalgae-harvesting method.