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Here we reported a self\u2010assembled living microreactor that encapsulated microcystin\u2010degrading bacteria within a biochar\u2010reinforced double\u2010network hydrogel, enabling integrated molecular sieving, adsorption, and enzymatic degradation. The system exhibited size\u2010 and charge\u2010selective removal of microcystin over coexisting organic matters, while maintaining high degradation efficiency under harsh stress conditions, including pH (5\u22129), inorganic ions (10\u2212200\u00a0mg\/L), and natural organic matters (5\u221220\u00a0mg\/L). The microreactor demonstrated excellent mechanical stability, negligible cell leakage, and high bioactivity, and achieved nearly complete removal of microcystin\u2010LR during five repeated operation cycles and continuous biofiltration in environmental water, confirming its scalable application potential. Mechanistic investigations revealed a cascade process involving shell\u2010confined molecular sieving, adsorption\u2010mediated toxin enrichment on biochar, and localized biodegradation within the living core. This work establishes a generalizable design paradigm for programmable living materials, offering new opportunities for selective biodegradation and remediation in complex aqueous systems.<\/jats:p>","DOI":"10.1002\/smll.74690","type":"journal-article","created":{"date-parts":[[2026,7,17]],"date-time":"2026-07-17T10:24:30Z","timestamp":1784283870000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Self\u2010Assembled Living Microreactors for Selective Microcystin Removal via Cascade Sieving, Adsorption and Biodegradation"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9800-3212","authenticated-orcid":false,"given":"Lixun","family":"Zhang","sequence":"first","affiliation":[{"name":"Guangdong Provincial Engineering Technology Research Center for Urban Water Cycle and Water Environment Safety Institute of Environment and Ecology, Shenzhen International Graduate School Tsinghua University  Shenzhen P. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shengyin","family":"Tang","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Engineering Technology Research Center for Urban Water Cycle and Water Environment Safety Institute of Environment and Ecology, Shenzhen International Graduate School Tsinghua University  Shenzhen P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sunny","family":"Jiang","sequence":"additional","affiliation":[{"name":"Department of Civil and Environmental Engineering University of California  Irvine California USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuntao","family":"Guan","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Engineering Technology Research Center for Urban Water Cycle and Water Environment Safety Institute of Environment and Ecology, Shenzhen International Graduate School Tsinghua University  Shenzhen P. R. 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