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Yet the single operation mode and insufficient on\/off ratio extremely restrict the ultimate device performance. Here, we design and construct a high\u2010order superlattice\u2010based memristor by rolling up oxide\/TMDCs heterostructures, which exhibits tunable resistive switching polarity and a high on\/off ratio. Four types of heterostructures are created via fine\u2010controlled oxygen plasma to in situ oxidize the top few layers into uniform transition metal oxide. Capillary forces in organic reagents are utilized to drive these heterostructures to spontaneously roll up. The as\u2010formed high\u2010order oxide\/TMDCs superlattices with alternately stacked TMDCs and oxides are clearly resolved by the cross\u2010section scanning transmission electron microscope and corresponding elemental mappings. With pre\u2010set oxide layers supplying mobile oxygen atoms, bipolar resistive switching of the high\u2010order superlattice\u2010based memristors is realized in vertical tunneling current measurements. In contrast, when the top and bottom electrodes are arranged in an interleaved configuration, the spatial confinement of conductive filaments converts the switching behavior into a unipolar mode. Furthermore, this polarity\u2010tunable memristor exhibits an outstanding on\/off ratio of approximately 10\n                    <jats:sup>7<\/jats:sup>\n                    and a robust multilevel resistance performance. Our work opens a new avenue for the fundamental design of high\u2010performance and multimodal memristors.\n                  <\/jats:p>","DOI":"10.1002\/adma.202522853","type":"journal-article","created":{"date-parts":[[2026,6,16]],"date-time":"2026-06-16T07:19:21Z","timestamp":1781594361000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Rolling Up Transition Metal Chalcogenides\/Oxide Heterostructures Enables Polarity\u2010Tunable and High\u2010Switchable Memristors"],"prefix":"10.1002","volume":"38","author":[{"given":"Xiaofan","family":"Wang","sequence":"first","affiliation":[{"name":"Key Laboratory for Intelligent Nano Materials and Devices of Ministry of Education State Key Laboratory of Mechanics and Control of Mechanical Structures and Institute for Frontier Science Nanjing University of Aeronautics and Astronautics  Nanjing 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Education State Key Laboratory of Mechanics and Control of Mechanical Structures and Institute for Frontier Science Nanjing University of Aeronautics and Astronautics  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinguo","family":"Liu","sequence":"additional","affiliation":[{"name":"Key Laboratory for Intelligent Nano Materials and Devices of Ministry of Education State Key Laboratory of Mechanics and Control of Mechanical Structures and Institute for Frontier Science Nanjing University of Aeronautics and Astronautics  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kun","family":"Yu","sequence":"additional","affiliation":[{"name":"National Laboratory of Solid State Microstructures Jiangsu Key Laboratory for Nanotechnology School of Physics Collaborative Innovation Center of Advanced Microstructures Nanjing University  Nanjing 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Education State Key Laboratory of Mechanics and Control of Mechanical Structures and Institute for Frontier Science Nanjing University of Aeronautics and Astronautics  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rong","family":"Rong","sequence":"additional","affiliation":[{"name":"Key Laboratory for Intelligent Nano Materials and Devices of Ministry of Education State Key Laboratory of Mechanics and Control of Mechanical Structures and Institute for Frontier Science Nanjing University of Aeronautics and Astronautics  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Libo","family":"Gao","sequence":"additional","affiliation":[{"name":"National Laboratory of Solid State Microstructures Jiangsu Key Laboratory for Nanotechnology School of Physics Collaborative Innovation Center of Advanced Microstructures Nanjing University  Nanjing 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