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However, timely detection remains challenging due to limitations in current point\u2010of\u2010care technologies. This study reveals that organic electrochemical transistors that include PEDOT:PSS\u00a0as the channel material exhibit inherent sensitivity to free bilirubin \u2010 but only when paired with polarizable gate electrodes (Au, Pt, glassy carbon). Intriguingly, this response is abolished with non\u2010polarizable Ag\/AgCl gates, highlighting the pivotal role of electrode polarizability in bilirubin detection. Furthermore, the drain\u2010source current changing direction is modulated by operational parameters, suggesting complex interfacial dynamics between bilirubin and channel material. Through systematic investigation, we demonstrate that this sensitivity persists for human serum albumin\u2010bound bilirubin, a clinically relevant complex, and elucidate the redox mechanisms underlying signal transduction via cyclic voltammetry. Our work not only decouples the influence of gate materials and measurement conditions on device performance but also establishes a foundational framework for designing high\u2010precision bilirubin sensors, paving the way for transformative diagnostic devices that address critical gaps in neonatal care through miniaturized, low\u2010power platforms capable of real\u2010time bilirubin monitoring in both clinical and resource\u2010limited settings.<\/jats:p>","DOI":"10.1002\/adhm.202502481","type":"journal-article","created":{"date-parts":[[2025,8,8]],"date-time":"2025-08-08T05:31:07Z","timestamp":1754631067000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Bilirubin Sensing Using Organic Electrochemical Transistors: Role of Gate Materials and Operational Parameters"],"prefix":"10.1002","volume":"14","author":[{"given":"Yunjia","family":"Song","sequence":"first","affiliation":[{"name":"Department of Medicine Solna Division of Dermatology and Venereology Karolinska Institutet  Stockholm 17177 Sweden"},{"name":"Centre for Molecular Medicine Karolinska University Hospital  Stockholm 17176 Sweden"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sihui","family":"Xu","sequence":"additional","affiliation":[{"name":"Department of Medicine Solna Division of Dermatology and Venereology Karolinska Institutet  Stockholm 17177 Sweden"},{"name":"Centre for Molecular Medicine Karolinska University Hospital  Stockholm 17176 Sweden"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6858-9638","authenticated-orcid":false,"given":"Onur","family":"Parlak","sequence":"additional","affiliation":[{"name":"Department of Medicine Solna Division of Dermatology and Venereology Karolinska Institutet  Stockholm 17177 Sweden"},{"name":"Centre for Molecular Medicine Karolinska University Hospital  Stockholm 17176 Sweden"},{"name":"Center for the Advancement of Integrated Medical and Engineering Sciences Karolinska Institutet and KTH Royal Institute of Technology  Stockholm 10044 Sweden"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,8,7]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1001\/jama.1899.92450730001001"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1542\/pir.15.11.422"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1007\/s12098-019-02856-0"},{"key":"e_1_2_8_4_1","first-page":"599","volume":"65","author":"Porter M. 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