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Bioceramics such as calcium silicate (Ca-Si), have gained a lot of interest in the biomedical field due to their strength, osteogenesis capability, mechanical stability, and biocompatibility. As such, these materials are excellent candidates to promote bone and tissue regeneration along with treating bone cancer. Bioceramic scaffolds, functionalized with appropriate materials, can achieve desirable photothermal effects, opening up a bifunctional approach to osteosarcoma treatments—simultaneously killing cancerous cells while expediting healthy bone tissue regeneration. At the same time, they can also be used as vehicles and cargo structures to deliver anticancer drugs and molecules in a targeted manner to tumorous tissue. However, the traditional synthesis routes for these bioceramic scaffolds limit the macro-, micro-, and nanostructures necessary for maximal benefits for photothermal therapy and drug delivery. Therefore, a different approach to formulate bioceramic scaffolds has emerged in the form of 3D printing, which offers a sustainable, highly reproducible, and scalable method for the production of valuable biomedical materials. Here, calcium silicate (Ca-Si) is reviewed as a novel 3D printing base material, functionalized with highly photothermal materials for osteosarcoma therapy and drug delivery platforms. Consequently, this review aims to detail advances made towards functionalizing 3D-printed Ca-Si and similar bioceramic scaffold structures as well as their resulting applications for various aspects of tumor therapy, with a focus on the external surface and internal dispersion functionalization of the scaffolds.