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While biocatalysis offers a promising approach for sustainable and effective plastic degradation, the inherently low solubility of plastics in aqueous systems severely limits the efficiency of enzymatic reactions. To address this issue, we developed a biocompatible polymer coating strategy to engineer living cell surfaces, enabling the stabilization of Pickering emulsions for over 192 h and significantly enhancing plastic accessibility to biocatalysts. Leveraging this platform, <jats:italic>Escherichia coli<\/jats:italic> (<jats:italic>E. coli<\/jats:italic>) cells containing overexpressed <jats:italic>Candida antarctica<\/jats:italic> Lipase B performed well by dispersing at the emulsion interface of water and toluene, facilitating the efficient biodegradation of polycarbonate (PC) plastics. Under optimized reaction conditions (pH 9, 45\u00a0\u00b0C), this Pickering emulsion system achieved efficient PC degradation, producing up to 4.5\u00a0m<jats:sc>m<\/jats:sc> bisphenol A within 72 h\u2014far exceeding the performance of biphasic systems using native <jats:italic>E. coli<\/jats:italic> cells. The findings highlight the transformative potential of surface\u2010engineered whole\u2010cell catalysts in addressing environmental challenges, particularly plastic waste remediation.<\/jats:p>","DOI":"10.1002\/smll.202504376","type":"journal-article","created":{"date-parts":[[2025,5,24]],"date-time":"2025-05-24T15:47:54Z","timestamp":1748101674000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Pickering Emulsion Biocatalysis with Engineered Living Cells for Degrading Polycarbonate Plastics"],"prefix":"10.1002","volume":"21","author":[{"given":"Shan","family":"Wang","sequence":"first","affiliation":[{"name":"Department of Physics Chemistry and Pharmacy University of Southern Denmark  Campusvej 55 Odense 5230 Denmark"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Zhimin","family":"Gong","sequence":"additional","affiliation":[{"name":"Department of Physics Chemistry and Pharmacy University of Southern Denmark  Campusvej 55 Odense 5230 Denmark"},{"name":"School of Geographic Information and Tourism Chuzhou University  Chuzhou 239000 P.R. 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