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Extending the \u03c0\u2010conjugation of end groups is an effective strategy to tune molecular energy levels, enhance optical absorption, and optimize intermolecular packing, yet the effects on both photovoltaic and photocatalytic performance remains insufficiently explored. NFAs featuring an indanone\u2010based central core have demonstrated excellent photovoltaic and photocatalytic performance. In this study, we design two novel NFAs, NQF\u2010F and NQF\u2010FN, derived from a common indanone\u2010based NQF backbone, incorporating phenyl\u2010 and naphthyl\u2010fuzed indanone end groups. The extended \u03c0\u2010conjugation in NQF\u2010FN results in broader absorption, improved charge transport, and a higher PCE of 17.06%, outperforming NQF\u2010F (16.29%). More importantly, PM6:NQF\u2010FN\u2010based photocatalysts achieve a hydrogen evolution rate of 217.5\u2009mmol\u2009h\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    with only 10\u2009wt% Pt, compared to 214.4\u2009mmol\u2009h\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    for PM6:NQF\u2010F, despite a fourfold reduction in Pt content. These findings underscore the potential of end\u2010group conjugation extension to enhance both photovoltaic and photocatalytic performance while reducing reliance on precious metals, providing critical design insights for multifunctional NFAs in energy conversion applications.\n                  <\/jats:p>","DOI":"10.1002\/cssc.202502733","type":"journal-article","created":{"date-parts":[[2026,4,26]],"date-time":"2026-04-26T23:58:41Z","timestamp":1777247921000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Tailoring End\u2010Group \u03c0\u2010Conjugation in Nonfullerene Acceptors for Enhanced Photovoltaic and Photocatalytic Hydrogen Evolution"],"prefix":"10.1002","volume":"19","author":[{"given":"Hongyan","family":"Zhang","sequence":"first","affiliation":[{"name":"School of Materials Science &amp; Engineering Tianjin Key Laboratory for Photoelectric Materials and Devices Key Laboratory of Display Materials &amp; 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