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The fracture proneness of molecular ferroelectrics under mechanical loading precludes their applications as flexible sensors in bulk crystalline form. Here, self\u2010powered flexible mechanical sensors prepared from the facile deposition of molecular ferroelectric [C(NH\n                    <jats:sub>2<\/jats:sub>\n                    )\n                    <jats:sub>3<\/jats:sub>\n                    ]ClO\n                    <jats:sub>4<\/jats:sub>\n                    onto a porous polyurethane (PU) matrix are reported. [C(NH\n                    <jats:sub>2<\/jats:sub>\n                    )\n                    <jats:sub>3<\/jats:sub>\n                    ]ClO\n                    <jats:sub>4<\/jats:sub>\n                    \u2010PU is capable of detecting pressure of 3\u00a0Pa and strain of 1% that are hardly accessible by the state\u2010of\u2010the\u2010art piezoelectric, triboelectric, and piezoresistive sensors, and presents the ability of sensing multimodal mechanical forces including compression, stretching, bending, shearing, and twisting with high cyclic stability. This scaling analysis corroborated with computational modeling provides detailed insights into the electro\u2010mechanical coupling and establishes rules of engineering design and optimization for the hybrid sponges. Demonstrative applications of the [C(NH\n                    <jats:sub>2<\/jats:sub>\n                    )\n                    <jats:sub>3<\/jats:sub>\n                    ]ClO\n                    <jats:sub>4<\/jats:sub>\n                    \u2010PU array suggest potential uses in interactive electronics and robotic systems.\n                  <\/jats:p>","DOI":"10.1002\/adma.202104107","type":"journal-article","created":{"date-parts":[[2021,9,12]],"date-time":"2021-09-12T14:07:01Z","timestamp":1631455621000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":73,"title":["Molecular Ferroelectric\u2010Based Flexible Sensors Exhibiting Supersensitivity and Multimodal Capability for Detection"],"prefix":"10.1002","volume":"33","author":[{"given":"Wenru","family":"Li","sequence":"first","affiliation":[{"name":"School of Optical and Electronic Information, and Wuhan National Laboratory for Optoelectronics Huazhong University of 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