Osteosarcoma has poor prognosis owing to its aggressive metastasis and high recurrence rates due to residualcancer cells which are common even after surgical resection. In addition, for irregular defects, site-specific designis essential to ensure anatomical conformity. Consequently, a critical demand exists for a theragenerative approachthat simultaneously provides structural reconstruction and functional eradication of residual cancer cells. Herein,we present a patient-specific 3D-printed theragenerative polyetheretherketone (PEEK) scaffold integrated withbiofunctional 2D molybdenum disulfide (MoS2) to impart enhanced bioactivity and dual-phototherapy. 2Dmonolayer MoS2 synthesized via nanoseed-initiated atmospheric pressure chemical vapor deposition (APCVD) wassubsequently integrated onto the 3D-printed PEEK through a polymer-assisted transfer process. The fabricated 2DMoS2-conformal 3D-printed PEEK scaffold (MoS2@PEEK) enabled simultaneous photothermal and photodynamictherapy via the intrinsic photoresponsive properties MoS2. Under dual-wavelength irradiation, this combinedphototherapy effectively induced pronounced cancer cell apoptosis and exhibited antibacterial activity throughthe synergistic effects of localized hyperthermia and reactive oxygen species generation. In contrast, under thesame photothermal stimulation, pre-osteoblasts and vascular endothelial cells exhibited enhanced attachment,proliferation, and differentiation. Therefore, this theragenerative system represents a promising patient-specificplatform for simultaneous tumor suppression, infection control, and bone regeneration after osteosarcomaresection.