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A multiferroic composite membrane, combining PVDF piezoelectric polymer and nickel ferrite (NFO) nanofibers, was successfully fabricated and studied as an active material layer in multifunctional devices designed to harvest both mechanical and magnetic energy. Optimization of the manufacturing process ensured an even distribution of NFO fibers within the PVDF matrix, enhancing the crystallization of PVDF in the electroactive βphase. The resulting PVDF/NFO multiferroic films exhibited both piezoelectric and magnetic properties, along with a pronounced magnetoelectric (ME) effect. In a structure comprising Al/PVDF-NFO/PDMS/Al, the device operated as a piezoelectric generator (PEG) under a pressing force of 0.5 MPa, achieving a maximum output power density of 14.7 μW cm−12with a peak-to-peak voltage of 12.2 V. When subjected to an AC magnetic field of 20 Oe at 50 Hz, the device functioned as a magneto-mechano-electrical (MME) generator, producing a sinusoidal waveform voltage of 486 mV. The cost-effective and easily integrable PVDF/NFO composite membrane presents promising opportunities for developing flexible, self-powered smart sensors for human health monitoring systems and implantable biomedical devices.