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Various bifunctional scaffolds have recently been developed to address the reconstruction of tumor‐initiated bone defects. Such scaffolds are usually composed of a near‐infrared (NIR) photothermal conversion agent and a conventional bone scaffold for photothermal therapy (PTT) and long‐term bone regeneration. However, the reported photothermal conversion agents are mainly restricted to the first biological window (NIR‐I) with intrinsic poor tissue penetration depth. Also, most of these agents are non‐bioactive materials, which induced potential systemic side toxicity after implantation. Herein, a NIR‐II photothermal conversion agent (Wesselsite [SrCuSi4O10] nanosheets, SC NSs) with tremendous osteogenic and angiogenic bioactivity, is rationally integrated with polycaprolactone (PCL) via 3D printing. The as‐designed 3D composite scaffolds not only trigger osteosarcoma ablation through NIR‐II light generated extensive hyperthermia, but also promote in vitro cellular proliferation and osteogenic differentiation of rat bone marrow mesenchymal stem cells (rBMSCs) and human umbilical vein endothelial cells (HUVECs), respectively, and the ultimate enhancement of vascularized bone regeneration in vivo owing to the controlled and sustained release of bioactive ions (Sr, Cu, and Si). The authors' study provides a new avenue to prepare multifunctional bone scaffolds based on therapeutic bioceramics for repairing tumor‐induced bone defects. [ABSTRACT FROM AUTHOR]

[Display omitted] • A facile strategy was developed for shape memory composite (SMC). • CaSiCu 4 O 10 (CUP) nanosheets exhibited good NIR-II photothermal activity. • SMC with CUP offered remote actuation and enhanced tissue reconstruction. • The release of Cu2+ and SiO 4 4- ions from CUP could accelerate wound healing. Near-infrared (NIR) light-responsive shape-memory composites have shown great potential in various biomedical applications due to their amazing remote actuation property. However, most of them are bioinert and restricted in NIR-I biological window. Here, we developed a new biodegradable NIR-II-responsive shape memory composite by the incorporation of CaSiCu 4 O 10 nanosheets (CUP NSs) into shape memory polymer of poly (D, L-lactide-co-trimethylene carbonate) (PDLLA-co-TMC, denoted as PT). The as-prepared CUP/PT composites possessed outstanding shape memory performance upon low power NIR-II laser irradiation (1064 nm, 0.4 W·cm−2), offering the possibility of deep-tissue applications. Moreover, due to the sustained release of bioactive Cu2+ and SiO 4 4- ions, the composites exhibited strong stimulation of angiogenesis both in vitro and in vivo. Our work demonstrated the promising potential of CUP/PT composites as NIR-II light-responsive biomaterials with enhanced tissue reconstruction ability, especially for wound healing. [ABSTRACT FROM AUTHOR]