This study comprehensively analyzed green nanomagnetic iron oxide particles (GNMIOPs) synthesized using a green method, investigating their size, shape, crystallinity, aggregation, phase portions, stability, and magnetism. The influence of pH and washing solvents on the magnetic properties of the nanoparticles and their incorporation into PCL membranes was examined for biomedical applications. Polyphenols were utilized at different pH values (1.2, 7.5, and 12.5), with washing being performed using either ethanol or water. Characterization techniques, including XRD, SEM, TEM, FTIR, and VSM, were employed, along with evaluations of stability, magnetic properties, and antioxidant activity. The findings indicate that both pH levels and the washing process exert a substantial influence on several properties of NMIOPs. The particle sizes ranged from 6.6 to 23.5 nm, with the smallest size being observed for GNMIOPs prepared at pH 12.5. Higher pH values led to increased crystallinity, cubic Fe3O4 fractions, and reduced crystalline anisotropy. SEM and TEM analyses showed pH-dependent morphological variations, with increased aggregation being observed at lower pH values. GNMIOPs displayed exceptional magnetic behavior, with the highest saturation magnetization being observed in GNMIOPs prepared at pH 7.5 and 12.5 and subsequently washed with ethanol. The zeta potential measurements indicated a stability range for GNMIOPs spanning from −31.8 to −41.6 mV, while GNMIOPs synthesized under high-pH conditions demonstrated noteworthy antioxidant activity. Furthermore, it was explored how pH and washing solvent affected the morphology, roughness, and magnetic properties of GNMIOP-infused nanofiber membranes. SEM showed irregularities and roughness due to GNMIOPs, varying with pH and washing solvent. TEM confirmed better dispersion with ethanol washing. The magnetic response was stronger with ethanol-washed GNMIOPs, highlighting the influence of pH and washing solvent on membrane characteristics.