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Malignant bone tumor is one of the major bone diseases. The treatment of such a bone disease typically requires the removal of bone tumor and regeneration of tumor‐initiated bone defects simultaneously. To address this issue, it is required that implanted biomaterials should combine the bifunctions of both therapy and regeneration. In this work, a bifunctional graphene oxide (GO)‐modified β‐tricalcium phosphate (GO‐TCP) composite scaffold combining a high photothermal effect with significantly improved bone‐forming ability is prepared by 3D‐printing and surface‐modification strategies. The prepared GO‐TCP scaffolds exhibit excellent photothermal effects under the irradiation of 808 nm near infrared laser (NIR) even at an ultralow power density of 0.36 W cm−2, while no photothermal effects are observed for pure β‐TCP scaffolds. The photothermal temperature of GO‐TCP scaffolds can be effectively modulated in the range of 40–90 °C by controlling the used GO concentrations, surface‐modification times, and power densities of NIR. The distinct photothermal effect of GO‐TCP scaffolds induces more than 90% of cell death for osteosarcoma cells (MG‐63) in vitro, and further effectively inhibits tumor growth in mice. Meanwhile, the prepared GO‐TCP scaffolds possess the improved capability to stimulate the osteogenic differentiation of rabbit bone mesenchymal stem cells (rBMSCs) by upregulating bone‐related gene expression, and significantly promote new bone formation in the bone defects of rabbits as compared to pure β‐TCP scaffolds. These results successfully demonstrate that the prepared GO‐TCP scaffolds have bifunctional properties of photothermal therapy and bone regeneration, which is believed to pave the way to design and fabricate novel implanting biomaterials in combination of therapy and regeneration functions.

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Grape-seed extracts contain rich flavonoids with oligomeric proanthocyanidins (OPC). In this study, OPC containing hydrogel scaffolds can function as a natural photothermal agent for melanoma therapy and bioactive biomaterial for wound healing. Inspired by grapeseed extracts, OPC were explored as a photothermal agent and endowed the hydrogel scaffolds with excellent and controlled photothermal ability. The rheological property of the hydrogel scaffolds responded to irradiation time of near infrared (NIR) laser, and OPC contents. The compressive mechanical property of the hydrogel scaffolds was well modulated by NIR laser irradiation with different impact durations. The controlled high temperature induced by OPC-containing hydrogel scaffolds under NIR laser irradiation could effectively kill melanoma cells and suppress tumor growth. In addition, OPC-containing hydrogel scaffolds supported the proliferation and migration of human dermal fibroblasts and human umbilical vein endothelial cells, as well as obviously promoted angiogenesis and skin regeneration in both tumor-caused and chronic wounds. Therefore, OPC-containing hydrogel scaffolds possessed controlled photothermal, rheological, and compressive mechanical properties under NIR laser stimuli, as well as excellent biocompatibility and bioactivity for melanoma therapy and wound healing.