A strontium-containing piezoelectric biofilm was developed to promote dentin tissue regeneration. The biofilm, composed of P(VDF-TrFE) with 2 wt% SrCl₂, exhibits high flexibility, biocompatibility, and a large piezoelectric coefficient (d₃₃ ≈ 14 pC N⁻¹). It generates an electric microenvironment that recruits dental pulp stem cells (DPSCs) and promotes their differentiation into odontoblasts. Strontium ions are gradually released, further enhancing dentin regeneration. In vivo experiments showed that the biofilm effectively induces dentin tissue formation in large animal models over three months. The biofilm's piezoelectric properties and strontium release synergistically promote DPSC odonto-differentiation and mineralization, leading to new dentin tissue formation. The biofilm also supports neovascularization and has minimal adverse effects, as demonstrated by electric pulp testing. The study highlights the therapeutic potential of the piezoelectric biofilm in clinical dentin tissue repair. The biofilm's properties, including its piezoelectric response, biocompatibility, and controlled strontium release, make it a promising candidate for dentin regeneration. The results suggest that the biofilm can be used to treat dentin defects and pulp exposure, offering a novel approach to regenerate dentin tissue in clinical settings.A strontium-containing piezoelectric biofilm was developed to promote dentin tissue regeneration. The biofilm, composed of P(VDF-TrFE) with 2 wt% SrCl₂, exhibits high flexibility, biocompatibility, and a large piezoelectric coefficient (d₃₃ ≈ 14 pC N⁻¹). It generates an electric microenvironment that recruits dental pulp stem cells (DPSCs) and promotes their differentiation into odontoblasts. Strontium ions are gradually released, further enhancing dentin regeneration. In vivo experiments showed that the biofilm effectively induces dentin tissue formation in large animal models over three months. The biofilm's piezoelectric properties and strontium release synergistically promote DPSC odonto-differentiation and mineralization, leading to new dentin tissue formation. The biofilm also supports neovascularization and has minimal adverse effects, as demonstrated by electric pulp testing. The study highlights the therapeutic potential of the piezoelectric biofilm in clinical dentin tissue repair. The biofilm's properties, including its piezoelectric response, biocompatibility, and controlled strontium release, make it a promising candidate for dentin regeneration. The results suggest that the biofilm can be used to treat dentin defects and pulp exposure, offering a novel approach to regenerate dentin tissue in clinical settings.