Radiosensitizers　potentiate　the　radiotherapy　effect　while　effectively　reducing　the　damage　to　healthy　tissues.　However,　limited　sample　accumulation　efficiency　and　low　radiation　energy　deposition　in　the　tumor　significantly　reduce　the　therapeutic　effect.　Herein,　we　developed　multifunctional　photocatalysis-powered　dandelion-like　nanomotors　composed　of　amorphous　TiO2　components　and　Au　nanorods　(∼93　nm　in　length　and　∼16　nm　in　outer　diameter)　by　a　ligand-mediated　interface　regulation　strategy　for　NIR-II　photoacoustic　imaging-guided　synergistically　enhanced　cancer　radiotherapy.　The　non-centrosymmetric　nanostructure　generates　stronger　local　plasmonic　near-fields　close　to　the　Au-TiO2　interface.　Moreover,　the　Au-TiO2　Schottky　heterojunction　greatly　facilitates　the　separation　of　photogenerated　electron-hole　pairs,　enabling　hot　electron　injection,　finally　leading　to　highly　efficient　plasmon-enhanced　photocatalytic　activity.　The　nanomotors　exhibit　superior　motility　both　in　vitro　and　in　vivo,　propelled　by　H2　generated　via　NIR-catalysis　on　one　side　of　the　Au　nanorod,　which　prevents　them　from　returning　to　circulation　and　effectively　improves　the　sample　accumulation　in　the　tumor.　Additionally,　a　high　radiation　dose　deposition　in　the　form　of　more　hydroxyl　radical　generation　and　glutathione　depletion　is　authenticated.　Thus,　synergistically　enhanced　radiotherapeutic　efficacy　is　achieved　in　both　a　subcutaneous　tumor　model　and　an　orthotopic　model.　©　2022　The　Royal　Society　of　Chemistry.