Bipolar Metal Flexible Electrospun Fibrous Membrane Based on Metal–Organic Framework for Gradient Healing of Tendon‐to‐Bone Interface Regeneration

Abstract Metal ions play a significant role in tissue repair, with widely application in clinical treatment. However, the therapeutic effect of metal ions is always limited due to metabolization and narrow repair capability. Here, a bipolar metal flexible electrospun fibrous membrane based on a metal–organic framework (MOF), which is bioinspired by the gradient structure of the tendon‐to‐bone interface, with a combination of regulating osteoblasts differentiation and angiogenesis properties, is constructed successfully by a continuous electrospinning technique and matching the longitudinal space morphology for synchronous regeneration. Furthermore, the MOF, acting as carriers, can not only achieve the sustainable release of metal ions, but promote the osteogenesis and tenogenesis on the scaffold. The in vitro data show that this novel hierarchical structure can accelerate the tenogenesis, the biomineralization, and angiogenesis. Moreover, in the in vivo experiment, the flexible fibrous membrane can promote tendon and bone tissue repair, and fibrocartilage reconstruction, to realize the multiple tissue synchronous regeneration at the damaged tendon‐to‐bone interface. Altogether, this newly developed bipolar metal flexible electrospun fibrous membrane based on a MOF, as a new biomimetic flexible scaffold, has great potential in reconstruct the tissue damage, especially gradient tissue damage.