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Despite significant advances driven by innovations in materials, structures, hardware, and algorithms, conventional design approaches that focus on optimizing individual hierarchies have inherent performance trade-offs, limiting further development. This review contends that future performance enhancements can no longer rely solely on breakthroughs in separate components. Still, it must adopt a new co-design paradigm spanning the \u201cmaterials\u2013structure\u2013hardware\u2013algorithm\u201d hierarchy. In this review, we systematically organized the research landscape and representative advances across these four key hierarchies, analyzed the importance and recent breakthroughs in hierarchical synergy, and established a forward-looking theoretical framework to foster innovation and development in the field of flexible sensing.<\/jats:p>","DOI":"10.1007\/s40820-026-02274-w","type":"journal-article","created":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T09:11:15Z","timestamp":1786353075000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Materials\u2013Structure\u2013Hardware\u2013Algorithm Co-Driven Hierarchical Optimization for Flexible Sensors"],"prefix":"10.1007","volume":"19","author":[{"given":"Pengyu","family":"Zhu","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peng","family":"He","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinbo","family":"Pang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mark Hermann","family":"Rummeli","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hong","family":"Liu","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weijia","family":"Zhou","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rafael Gregorio","family":"Mendes","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuye","family":"Zhang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"297","published-online":{"date-parts":[[2026,8,10]]},"reference":[{"issue":"36","key":"2274_CR1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.ady0534","volume":"11","author":"C Li","year":"2025","unstructured":"C. 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