The fabrication of electrospun magnetoactive fibrous nanocomposite membranes based on the water-soluble and biocompatible poly(ethylene oxide) (PEO), the biocompatible and biodegradable poly(L-lactide) (PLLA) and preformed oleic acid-coated magnetite nanoparticles (OA.Fe3O4) is reported. Visualization of the membranes by electron microscopy techniques reveals the presence of continuous fibers of approximately 2 μm in diameter, with the magnetic nanoparticles being evenly distributed within the fibers, retaining at the same time their nanosized diameters (≈ 5 nm). Thermal gravimetric analysis measurements suggest that the magnetic nanoparticles embedded within the polymer fibers affect favorably the thermal stability of the membranes. Moreover, assessment of their magnetic characteristics by vibrating sample magnetometry discloses tunable superparamagnetic behavior at ambient temperature. For the first time, the biocompatibility and biodegradability of PEO/PLLA and the tunable magnetic activity of the OA.Fe3O4 are combined in the same drug delivery system, with N-acetyl-p-aminophenol (acetaminophen) as a proof-of-concept pharmaceutical. Furthermore, their heating ability under alternating current (AC) magnetic field conditions is evaluated using frequency of 110 kHz and corresponding magnetic field strength of 25 mT (19.9 kA/m). Consequently, these magnetoactive fibrous nanocomposites exhibit promising characteristics for future exploitation in magnetothermally triggered drug delivery.