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In this study, erythrocyte microreactors capable of prolonged hydrogen sulfide (H\u2082S) production for therapeutic vasodilation are developed. The microreactors are fabricated by encapsulating a pyridoxal 5\u2032\u2010phosphate\u2010polylysine (PLP\u2010PLys) complex into erythrocytes using a hypotonic swelling method. The optimized process achieved a loading efficiency of 61.5%, ensuring the uniform distribution of PLP\u2010PLys within the erythrocytes while maintaining structural integrity and cellular viability. Synthetic biocatalysis within these microreactors is initiated through a cascade reaction mediated by PLP\u2010PLys complex\u00a0and hemoglobin (Hb) upon exposure to L\u2010cysteine (L\u2010Cys). This system demonstrated efficient H\u2082S production with sustained kinetics, achieving peak concentrations of 6.2 \u00b5\n                    <jats:sc>m<\/jats:sc>\n                    after 180\u00a0min. The therapeutic potential of the microreactors is validated in vitro using isolated thoracic aortic rings. Upon L\u2010Cys exposure, the microreactors generated localized H\u2082S, inducing significant vasodilation, with a 39.17% reduction in vascular tension. Fluorescence imaging further confirmed H\u2082S production within blood vessels, highlighting the specificity and efficacy of the erythrocyte microreactors. This innovative platform offers a controlled, sustained strategy for gasotransmitter delivery, presenting promising applications in cardiovascular therapy and beyond.\n                  <\/jats:p>","DOI":"10.1002\/smll.202502208","type":"journal-article","created":{"date-parts":[[2025,6,1]],"date-time":"2025-06-01T22:11:48Z","timestamp":1748815908000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Synthetic Biocatalysis in Erythrocyte Microreactors for Gasotransmitter H\n                    <sub>2<\/sub>\n                    S Production and Vessel Vasodilation"],"prefix":"10.1002","volume":"21","author":[{"given":"Yuling","family":"Yan","sequence":"first","affiliation":[{"name":"College of Chemistry and Chemical Engineering State Key Laboratory of Chemo\/Biosensing and Chemometrics Hunan University  Changsha 410082 P. R. 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