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Physical unclonable functions (PUFs) exploit structural randomness to generate unique cryptographic responses, establishing hardware\u2010based security. However, conventional PUF architectures rely on static configurations to guarantee authentication reproducibility, and the intrinsic rigidity permits unauthorized reverse\u2010engineering without detectable traces. A tamper\u2010responsive physical unclonable function (TR\u2010PUF) platform is presented, integrating a high\u2010entropy source with a reactive two\u2010dimensional material interlayer to actively defend cryptographic keys. The entropy source relies on fingerprint\u2010like nanopatterns derived from thermodynamic fluctuations during block copolymer self\u2010assembly, while a reduced graphene oxide interlayer leverages out\u2010of\u2010plane chemical and mechanical sensitivity enabling device responsiveness to external intrusions. Systematic characterization confirms robust fundamental cryptographic performance, with near\u2010ideal uniqueness and uniformity. Also, the tamper\u2010responsive capability is demonstrated across three representative intrusion scenarios, where simulated high\u2010resolution probing, chemical, or mechanical attempts to access the internal architecture trigger spontaneous and irreversible key invalidation via localized degradation. Furthermore, broad applicability is validated through rigorous environmental survivability assessment under low Earth orbit simulated conditions, alongside seamless integration across diverse form factors. The autonomous hardware protection framework opens possibilities for securing electronic components across next\u2010generation hardware architectures in strategic fields like space missions and military applications.<\/jats:p>","DOI":"10.1002\/adma.75142","type":"journal-article","created":{"date-parts":[[2026,9,25]],"date-time":"2026-09-25T06:15:24Z","timestamp":1790316924000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Tamper\u2010Responsive Physical Unclonable Functions via Graphene\u2010Interlayered Block Copolymer Random Structures"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-6982-9016","authenticated-orcid":false,"given":"Gyu Hui","family":"Jo","sequence":"first","affiliation":[{"name":"Department of Organic Materials Engineering Chungnam National University  Daejeon Republic of Korea"},{"name":"Department of Materials Science and Engineering Chungnam National University  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