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In contrast, ultrasound\u2010driven polymerization offers deeper penetration but limited spatiotemporal control. To address these challenges, we pioneer the integration of piezo\u2010photocatalysis into ATRP by developing a donor\u2013acceptor (D\u2013A) metal\u2013organic framework (MOF) catalyst (B\u2010Zr\u2010C) via incorporating electron\u2010acceptor N\u2010(4\u2032\u2010carboxyphenyl)\u20101,8\u2010naphthalimide (CPNI) into NH\n                    <jats:sub>2<\/jats:sub>\n                    \u2010UiO\u201066, which enables synergistically enhanced piezoelectric polarization and exciton separation. Multiscale characterizations verify that the introduction of CPNI prolongs the charge\u2010separated state lifetime and effectively increases the polarity of the MOF, as evidenced by significant increases in the piezoelectric coefficient d\n                    <jats:sub>33<\/jats:sub>\n                    , piezoelectric potential difference, and dipole moment. Under blue light and ultrasound, the piezo\u2010photocatalytic copper\u2010mediated ATRP apparent rate constant of B\u2010Zr\u2010C(1:1) is \u223cfourfold higher than that under light alone, achieving high monomer conversion (&gt; 90%,\n                    <jats:italic>\u0110<\/jats:italic>\n                    &lt; 1.11) in seven polar solvents and even producing ultrahigh\u2010molecular\u2010weight (UHMW) polymers (\n                    <jats:italic>M<\/jats:italic>\n                    <jats:sub>n<\/jats:sub>\n                    \u00a0&gt; 1100 kg\u00b7mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    ,\n                    <jats:italic>\u0110<\/jats:italic>\n                    &lt; 1.30). The piezo\u2010photocatalytic system retains 64% conversion through a 1.5\u00a0mm chicken\u2010skin barrier (vs. &lt;\u00a010% for blue light alone), together with outstanding spatiotemporal controllability, chain\u2010end fidelity, and reusability.\n                  <\/jats:p>","DOI":"10.1002\/anie.1148889","type":"journal-article","created":{"date-parts":[[2026,9,26]],"date-time":"2026-09-26T11:57:58Z","timestamp":1790423878000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Molecularly Engineered Metal\u2013Organic Framework With Synergistically Boosting Piezoelectric Polarization and Exciton Directional Separation Enables Efficient Piezo\u2010Photocatalytic Atom Transfer Radical Polymerization"],"prefix":"10.1002","author":[{"given":"Bei","family":"Liu","sequence":"first","affiliation":[{"name":"College of Chemistry Northeast Normal University  Changchun P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junjun","family":"Liu","sequence":"additional","affiliation":[{"name":"College of Chemistry Northeast Normal University  Changchun P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,9,26]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2020.06.014"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.9b00744"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/acssuschemeng.5c10810"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/s43586\u2010024\u201000370\u2010y"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.1c00409"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.1c00603"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010026\u201072346\u20103"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202518707"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202424225"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202422975"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202524267"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.4c01286"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202575058"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202304942"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.eurpolymj.2025.113837"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.macromol.7b01597"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201206476"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.5c02889"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201901361"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1021\/acssuschemeng.5c14012"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202508062"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2023.123058"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.macromol.4c01764"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c22163"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202312697"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c07945"},{"key":"e_1_2_8_28_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202106308"},{"key":"e_1_2_8_29_1","doi-asserted-by":"publisher","DOI":"10.1039\/d1mh01973b"},{"key":"e_1_2_8_30_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2025.125507"},{"key":"e_1_2_8_31_1","doi-asserted-by":"publisher","DOI":"10.1021\/cg200636k"},{"key":"e_1_2_8_32_1","doi-asserted-by":"publisher","DOI":"10.1002\/cjoc.70384"},{"key":"e_1_2_8_33_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcis.2025.137561"},{"key":"e_1_2_8_34_1","doi-asserted-by":"publisher","DOI":"10.1002\/chem.201304431"},{"key":"e_1_2_8_35_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202425656"},{"key":"e_1_2_8_36_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202520491"},{"key":"e_1_2_8_37_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201058839\u20107"},{"key":"e_1_2_8_38_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.inorgchem.5b01593"},{"key":"e_1_2_8_39_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c07699"},{"key":"e_1_2_8_40_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcis.2024.09.052"},{"key":"e_1_2_8_41_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.mtchem.2026.103393"},{"key":"e_1_2_8_42_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2025.126259"},{"key":"e_1_2_8_43_1","doi-asserted-by":"publisher","DOI":"10.1039\/c9sc04249k"},{"key":"e_1_2_8_44_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202521184"},{"key":"e_1_2_8_45_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201067467\u20100"},{"key":"e_1_2_8_46_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.74769"},{"key":"e_1_2_8_47_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.201904259"},{"key":"e_1_2_8_48_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202101751"},{"key":"e_1_2_8_49_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010023\u201038402\u2010y"},{"key":"e_1_2_8_50_1","doi-asserted-by":"publisher","DOI":"10.1007\/s13203\u2010018\u20100192\u2010y"},{"key":"e_1_2_8_51_1","doi-asserted-by":"publisher","DOI":"10.1021\/ma400565k"},{"key":"e_1_2_8_52_1","doi-asserted-by":"publisher","DOI":"10.1021\/ma901094s"},{"key":"e_1_2_8_53_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8CS00259B"},{"key":"e_1_2_8_54_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.2c10251"},{"key":"e_1_2_8_55_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c10541"},{"key":"e_1_2_8_56_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.4018657"},{"key":"e_1_2_8_57_1","doi-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