Abstract Owing to the strong near-infrared (NIR) absorption and high photothermal conversion efficiency, two-dimensional molybdenum disulfide (MoS2) has been extensively explored as a photothermal agent for cancer therapy. Moreover, the high specific surface area renders MoS2 nanomaterials to be instinct drug nanocarriers for photothermal combination therapy including chemotherapy, photodynamic therapy, radiotherapy, and gene therapy. For treating the tumor-induced tissue defects after surgery, an emerging bifunctional scaffold has been developed by incorporating MoS2 nanomaterials into bioceramic matrix for tumor therapy and tissue regeneration. This chapter summarizes the recent progress in combating cancer with MoS2 nanomaterials (1) as therapeutic agents for photothermal monotherapy and synergistic therapy; (2) integrated into tissue engineering scaffolds for tumor therapeutic potential and simultaneously for enhanced tissue regeneration capacity. We also provide our personal insight into the challenges and perspectives for MoS2-based biomaterials toward further clinical applications.