Ultrasound‐Driven Dual Piezocatalytic–Electrical Scaffold Synergistically Promotes Osteoporotic Bone Healing

The regeneration of osteoporotic bone defects is severely hampered by compromised endogenous healing capacity, demanding advanced strategies that actively orchestrate pro‐osteogenic microenvironments. Here, we report an integrated, self‐powered osteo‐regenerative system that uniquely leverages a dual ultrasound‐responsive piezoelectric mechanism for synergistic therapy. The system features a bilayer architecture comprising a foundational calcium‐doped poly(L‐lactic acid) (PLLA@Ca) nanofibrous membrane, in which Ca 2+ doping multifunctionally enhances piezoelectric polarization, surface wettability, and osteogenic ion release, and an overlying ionically conductive hydrogel embedded with barium titanate (BTO) nanoparticles (Hydrogel@BTO). Under ultrasound‐induced mechanical stress, both PLLA@Ca and BTO generate robust piezoelectric potentials that create a potent electrical stimulation field, whereas BTO's piezocatalytic effect concurrently scavenges excessive reactive oxygen species (ROS), restoring redox homeostasis. These synergistic electrophysiological and chemical cues are efficiently propagated and amplified by the hydrogel's iontronic network, establishing an energy‐autonomous therapeutic niche at the defect site. In vitro, this system significantly upregulated key osteogenic signaling pathways and enhanced mineralization. In a preclinical osteoporotic rat model, it dramatically accelerated new bone formation, enhanced bone volume and trabecular density, and modulated osteoclast activity. This work presents an energy‐autonomous synergistic “piezocatalytic‐electrical” therapeutic strategy, opening a new avenue for developing intelligent biomaterials to treat challenging bone disorders.