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It is shown that the linear configuration of diacetylene moieties within conjugated acetylenic polymers (CAPs) induces a pronounced polarization of electron distribution, which imparts enhanced charge\u2010carrier mobility when compared to CAPs\u2019 networks featuring cross\u2010linked arrangements. Moreover, optimizing the intramolecular spacer between diacetylene moieties within the linear structure leads to the exceptional modulation of the band structures, specifically resulting in a downshifted valence band (VB) and rendering the two\u2010electron water oxidation pathway thermodynamically feasible for H<jats:sub>2<\/jats:sub>O<jats:sub>2<\/jats:sub> production. Consequently, the optimized CAPs with a linear configuration (LCAP\u20102), featuring spatially separated reduction centers (benzene rings) and oxidation centers (diacetylene moieties), exhibit a remarkable H<jats:sub>2<\/jats:sub>O<jats:sub>2<\/jats:sub> yield rate of 920.1\u00a0\u00b5mol g<jats:sup>\u22121<\/jats:sup> h<jats:sup>\u22121<\/jats:sup>, superior than that of the linear LCAP\u20101 (593.2\u00a0\u00b5mol g<jats:sup>\u22121<\/jats:sup> h<jats:sup>\u22121<\/jats:sup>) and the cross\u2010linked CCAP (433.4\u00a0\u00b5mol g<jats:sup>\u22121<\/jats:sup> h<jats:sup>\u22121<\/jats:sup>). The apparent quantum efficiency (AQE) and solar\u2010to\u2010chemical energy conversion (SCC) efficiency of LCAP\u20102 are calculated to be 9.1% (<jats:italic>\u03bb<\/jats:italic> = 420\u00a0nm) and 0.59%, respectively, surpassing the performance of most previously reported conjugated polymers.<\/jats:p>","DOI":"10.1002\/smll.202305004","type":"journal-article","created":{"date-parts":[[2023,8,31]],"date-time":"2023-08-31T04:36:10Z","timestamp":1693456570000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Rational Design of Conjugated Acetylenic Polymers Enables a Two\u2010Electron Water Oxidation Pathway for Enhanced Photosynthetic Hydrogen Peroxide Generation"],"prefix":"10.1002","volume":"20","author":[{"given":"Zhiquan","family":"Jin","sequence":"first","affiliation":[{"name":"Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province College of Environment Zhejiang University of Technology  Hangzhou Zhejiang 310032 P. 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