AbstractVital pulp therapy (VPT) is considered a conservative treatment for preserving pulp viability in caries‐induced dental pulp infections. However, bacterial contamination negatively affects dentine‐pulp complex repair. The common capping materials show limited antimicrobial effects against some microorganisms. To improve the VPT efficacy, capping materials with increased antibacterial properties and enhanced odontogenic and angiogenic activities are needed. Herein, a SrCuSi₄O₁₀/gelatin methacrylate(SC/Gel) composite hydrogel has been proposed for infected dental pulp treatment. SrCuSi₄O₁₀ (SC) is a microscale bioceramic composed of assembled multilayered nanosheets that possesses good near‐infrared photothermal conversion ability and multiple bioactivities due to sustained Sr²⁺, Cu²⁺, and SiO₃²⁻ ion release. It is shown that the SC/Gel composite hydrogel efficiently eliminates Streptococcus mutans and Lactobacillus casei and inhibits biofilm formation under photothermal heating, while the ion extract from SC promotes odontogenesis of rat dental pulp stem cells and angiogenesis of human umbilical vein endothelial cells. The as‐designed therapeutic effect of SC/Gel composite hydrogel‐mediated VPT has been proven in a rat dental pulp infection model and yielded improved dentine‐pulp complex repair compared with the commercially used iRoot® BP Plus. This study suggests that the SC/Gel composite hydrogel is a potential pulp‐capping material with improved effects on dentine−pulp complex repair in infected pulp.