Three-Dimensional Magnetoelectric Nanocomposite GelMA Hydrogels for Wireless Electrical Stimulation of Cardiac Cells

Bioelectrical cues are essential for cardiac function and regeneration, yet current electrostimulation strategies rely on invasive electrodes that limit spatial control and clinical translation. Here, we report magnetoelectric nanocomposite hydrogels that combine core-shell CoFe₂O₄@BiFeO₃ magnetoelectric nanoparticles (ME NPs) with a photo-cross-linked methacrylated gelatin (GelMA) network, enabling wireless electroactivity through externally applied magnetic fields within a soft, biomimetic three-dimensional scaffold. Structural and physicochemical analyses confirmed the successful synthesis of crystalline core-shell ME NPs with strong interfacial coupling, as demonstrated by transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and magnetic hysteresis measurements showing exchange bias effects. Homogeneous incorporation of ME NPs within GelMA produced highly porous and interconnected hydrogels, as revealed by scanning electron microscopy and microcomputed tomography. The presence of nanoparticles reduced equilibrium swelling and refined pore architecture, suggesting increased effective cross-linking density and nanoparticle-polymer interactions. Mechanical testing showed soft elastomeric behavior with compressive moduli compatible with cardiac tissue. Under dynamic magnetic stimulation, magnetoelectric hydrogels significantly enhanced cardiac cell viability, proliferation, and morphological organization compared with pristine GelMA controls. After 10 days, the metabolic activity of cells cultured on GelMA-ME NP hydrogels under stimulation was approximately 3-fold higher than that of unstimulated GelMA. These results demonstrate that magnetoelectric hydrogels provide an effective platform for wireless electrostimulation, offering promising opportunities for cardiac tissue engineering and implantable bioelectronic therapies without wired electrodes.