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Herein, we report a dual porphyrin\u2013sensitized TiO\n                    <jats:sub>2<\/jats:sub>\n                    platform for visible\u2010light\u2010driven CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction, integrating a Zn\u2010porphyrin photosensitizer with newly designed Fe\u2010porphyrin catalysts bearing urea\u2010based secondary\u2010sphere functionalities. These hydrogen\u2010bonding motifs promote CO\n                    <jats:sub>2<\/jats:sub>\n                    preorganization and stabilization of key reduced intermediates at the metal center. Systematic comparison of homogeneous and heterogeneous systems reveals a pronounced enhancement in activity and durability upon immobilization onto TiO\n                    <jats:sub>2<\/jats:sub>\n                    nanoparticles. Optimization studies demonstrate that catalytic activity is strongly governed by both sacrificial electron donor (SED) availability and proton concentration. Under anhydrous conditions, increased SED concentration boosts turnover numbers, while the introduction of controlled amounts of water enhances proton\u2010coupled electron transfer but ultimately compromises catalyst stability at higher concentrations. Under optimized conditions, the best\u2010performing assembly achieves turnover numbers (TONs) exceeding 15,000 after 96\u2009h of irradiation, representing, to the best of our knowledge, the highest reported TON for Fe\u2010porphyrin\u2010based dye\u2010sensitized photocatalytic systems (DSPs). These findings highlight the delicate balance between electron and proton management in dye\u2010sensitized architectures and provide key design principles for developing durable and efficient molecular\u2013semiconductor hybrids for solar\u2010driven CO\n                    <jats:sub>2<\/jats:sub>\n                    conversion.\n                  <\/jats:p>","DOI":"10.1002\/cssc.71128","type":"journal-article","created":{"date-parts":[[2026,10,6]],"date-time":"2026-10-06T17:59:08Z","timestamp":1791309548000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Dual Porphyrin Sensitized Photocatalytic System for Visible\u2010Light\u2010Driven CO\n                    <sub>2<\/sub>\n                    Reduction"],"prefix":"10.1002","volume":"19","author":[{"given":"Anna","family":"Katsari","sequence":"first","affiliation":[{"name":"Foundation for Research and Technology (FORTH) Institute of Electronic Structure and Laser (IESL)  Heraklion Greece"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2320-6672","authenticated-orcid":false,"given":"Emmanouil","family":"Nikoloudakis","sequence":"additional","affiliation":[{"name":"Foundation for Research and Technology (FORTH) Institute of Electronic Structure and Laser (IESL)  Heraklion Greece"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1237-9962","authenticated-orcid":false,"given":"Georgios","family":"Charalambidis","sequence":"additional","affiliation":[{"name":"Theoretical and Physical Chemistry Institute National Hellenic Research Foundation  Athens Greece"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0004-0081-7042","authenticated-orcid":false,"given":"Antonios","family":"Iliakis","sequence":"additional","affiliation":[{"name":"Foundation for Research and Technology (FORTH) Institute of Electronic Structure and Laser (IESL)  Heraklion Greece"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fabrice","family":"Odobel","sequence":"additional","affiliation":[{"name":"Universit\u00e9 de Nantes, CNRS, CEISAM UMR 6230  Nantes Cedex France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1908-8618","authenticated-orcid":false,"given":"Emmanuel","family":"Stratakis","sequence":"additional","affiliation":[{"name":"Foundation for Research and Technology (FORTH) Institute of Electronic Structure and Laser (IESL)  Heraklion Greece"},{"name":"Qingdao Innovation and Development Center Harbin Engineering University  Qingdao Shandong P.\u00a0R. 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