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The integration of photosensitizers (PSs) in localized drug delivery systems (DDSs), particularly in electrospun nanofibers, holds tremendous potential to overcome the drawbacks of their systemic administration. Exploring multilayer fibrous architectures provides a versatile therapeutic platform to design the next generation of localized DDS. In this work, localized implants for cancer treatment using PDT were developed using polyhydroxyalkanoate (PHA), chitosan (CS) and polyethylene oxide (PEO) as biopolymers and a porphyrin (Por) as PS, following two approaches: blended PHA\/Por electrospun microfibers and multilayered membranes (PHA\u2013Por\/CS\/PEO) produced by sequential electrospinning. The synthesized Por displayed higher cytotoxicity in light compared to dark against tumor cells. All the developed membranes were characterized regarding their morphology, wettability, absorption and fluorescence properties. PHA\u2013Por membranes exhibited overall uniform fibrous morphologies with successful Por incorporation. Nonetheless, they presented a highly hydrophobic surface, compromising the Por release and cell\u2013material interactions. In contrast, multilayer PHA\u2013Por\/CS\/PEO membranes demonstrated enhanced hydrophilicity and enabled sustained Por release. Upon light irradiation, these membranes induced a significantly greater inhibition of HeLa cell proliferation (29.61%) compared to dark conditions (6.21%), confirming their photodynamic activity.<\/jats:p>","DOI":"10.3390\/molecules31050842","type":"journal-article","created":{"date-parts":[[2026,3,4]],"date-time":"2026-03-04T16:17:31Z","timestamp":1772641051000},"page":"842","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Electrospun Fibrous Architectures for Localized Delivery of Photosensitizers in Cancer Therapy"],"prefix":"10.3390","volume":"31","author":[{"given":"C\u00e1tia V.","family":"Gomes","sequence":"first","affiliation":[{"name":"Centre for Textile Science and Technology (2C2T), University of Minho, 4800-058 Guimar\u00e3es, Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sofia M.","family":"Costa","sequence":"additional","affiliation":[{"name":"Centre for Textile Science and Technology (2C2T), University of Minho, 4800-058 Guimar\u00e3es, Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-6562-7516","authenticated-orcid":false,"given":"Jo\u00e3o S.","family":"Oliveira","sequence":"additional","affiliation":[{"name":"Centre for Textile Science and Technology (2C2T), University of Minho, 4800-058 Guimar\u00e3es, Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6801-4578","authenticated-orcid":false,"given":"Ricardo C.","family":"Calhelha","sequence":"additional","affiliation":[{"name":"Mountain Research Center (CIMO), Associated Laboratory for Sustainability and Technology in Inland Regions (LA SusTEC), Instituto Polit\u00e9cnico de Bragan\u00e7a, Campus de Santa Apol\u00f3nia, 5300-253 Bragan\u00e7a, Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1624-6825","authenticated-orcid":false,"given":"Leandro M. O.","family":"Louren\u00e7o","sequence":"additional","affiliation":[{"name":"Laborat\u00f3rio Associado para a Qu\u00edmica Verde (LAQV-REQUIMTE), Department of Chemistry, University of Aveiro, 3810-193 Aveiro, Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3303-6563","authenticated-orcid":false,"given":"Raul","family":"Fangueiro","sequence":"additional","affiliation":[{"name":"Centre for Textile Science and Technology (2C2T), University of Minho, 4800-058 Guimar\u00e3es, Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7862-4687","authenticated-orcid":false,"given":"Diana P.","family":"Ferreira","sequence":"additional","affiliation":[{"name":"Centre for Textile Science and Technology (2C2T), University of Minho, 4800-058 Guimar\u00e3es, Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"1968","published-online":{"date-parts":[[2026,3,3]]},"reference":[{"key":"ref_1","unstructured":"(2026, January 15). 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