Large　osseous　void,　postsurgical　neoplastic　recurrence,　and　slow　bone-cartilage　repair　rate　raise　an　imperative　need　to　develop　functional　scaffold　in　clinical　osteosarcoma　treatment.　Herein,　a　bionic　bilayer　scaffold　constituting　croconaine　dye-polyethylene　glycol@sodium　alginate　hydrogel　and　poly(L-lactide)/hydroxyapatite　polymer　matrix　is　fabricated　to　simultaneously　achieve　a　highly　efficient　killing　of　osteosarcoma　and　an　accelerated　osteochondral　regeneration.　First,　biomimetic　osteochondral　structure　along　with　adequate　interfacial　interaction　of　the　bilayer　scaffold　provide　a　structural　reinforcement　for　transverse　osseointegration　and　osteochondral　regeneration,　as　evidenced　by　upregulated　specific　expressions　of　collagen　type-I,　osteopontin,　and　runt-related　transcription　factor　2.　Meanwhile,　thermal　ablation　of　the　synthesized　nanoparticles　and　mitochondrial　dysfunction　caused　by　continuously　released　hydroxyapatite　induce　residual　tumor　necrosis　synergistically.　To　validate　the　capabilities　of　inhibiting　tumor　growth　and　promoting　osteochondral　regeneration　of　our　proposed　scaffold,　a　novel　orthotopic　osteosarcoma　model　simulating　clinical　treatment　scenarios　of　bone　tumors　is　established　on　rats.　Based　on　amounts　of　in　vitro　and　in　vivo　results,　an　effective　killing　of　osteosarcoma　and　a　suitable　osteal-microenvironment　modulation　of　such　bionic　bilayer　composite　scaffold　are　achieved,　which　provides　insightful　implications　for　photonic　hyperthermia　therapy　against　osteosarcoma　and　following　osseous　tissue　regeneration.