An　ideal　drug　delivery　platform　with　high　cell　selectivity,　drug　payload　capacity,　and　cellular　internalization　capability　is　usually　of　the　essence　for　targeted　cancer　chemotherapy.　Herein,　by　combining　palindromic　DNA　strands　with　a　targeting　aptamer　probe,　we　demonstrated　a　self-assembled　nanoscale　sea　urchin-shaped　structure　(called　aptamer-NSU)　as　a　multivalent　carrier　capable　of　executing　targeted　cancer　cell　imaging　and　drug　delivery.　The　DNA　nanostructure　is　composed　of　a　spherical　trunk　and　surface-confined　spines:　the　former　is　assembled　from　only　one　biotinylated　DNA　containing　four　different　palindrome　domains,　and　the　latter　is　a　biotinylated　aptamer　(Sgc8)　conjugated　to　the　trunk　surface　via　streptavidin-biotin　affinity　interaction.　The　spherical　trunk　can　densely　load　doxorubicin　(Dox),　and　the　surface-confined　Sgc8　probes　can　function　as　targeting　moieties　to　specifically　bind　to　target　cells　in　a　polyvalent-binding　fashion.　Atomic　force　microscopy　(AFM)　and　gel　electrophoresis　show　the　assembly　of　Sgc8-NSU.　The　confocal　fluorescence　imaging　demonstrates　that　fluorescently　labeled　Sgc8-NSU　can　specifically　image　CEM　cells.　Flow　cytometric　analyses　indicate　that　Sgc8-NSU　exhibits　the　multivalent　binding　effect,　achieving　the　significant　improvement　in　binding　affinity　and　selectivity　compared　with　free　Sgc8.　Moreover,　the　CCK-8　assay　confirmed　that　Dox-loaded　Sgc8-NSU　induces　an　enhanced　cellular　cytotoxicity　to　target　cancer　cells　but　not　to　negative　nontarget　cells.　The　developed　DNA　nanoplatform　is　expected　to　provide　a　valuable　insight　into　constructing　structural　DNA　nanotechnology-based　drug　delivery　nanovehicles　suitable　for　targeted　cancer　therapy.　©　2020　American　Chemical　Society.