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Although ligand engineering has been widely explored for the hydrogen evolution reaction (HER), few studies have treated ligand \u03c0\u2010conjugation area as a defined molecular variable and systematically examined its relationship with HER performance. Here, we use a conjugated\u2010ligand engineering strategy to systematically vary ligand \u03c0\u2010conjugation area while maintaining comparable metal coordination environments. Pyromellitic dianhydride (PMDA), naphthalene\u20101,4,5,8\u2010tetracarboxylic dianhydride (NTDA), and perylene\u20103,4,9,10\u2010tetracarboxylic dianhydride (PTCDA), featuring benzene\u2010, naphthalene\u2010, and perylene\u2010based aromatic cores with 6, 10, and 20 \u03c0 electrons, respectively, are used as precursors to the corresponding tetracarboxylate ligands to construct related Ni\u2010 and Co\u2010based MOFs with six\u2010coordinate metal centers. Across both metal series, increasing ligand \u03c0\u2010conjugation area consistently lowers overpotentials and Tafel slopes, decreases charge\u2010transfer resistance and mass\u2010transport\u2010related impedance, and increases electrochemically active surface area. This systematic ligand variation is accompanied by metal\u2010center binding\u2010energy shifts and bandgap narrowing. These results establish a clear structure\u2013performance relationship between ligand \u03c0\u2010conjugation area and HER performance across the investigated MOF series, highlighting conjugated\u2010ligand engineering as an effective strategy for MOF electrocatalyst design.<\/jats:p>","DOI":"10.1002\/smll.75945","type":"journal-article","created":{"date-parts":[[2026,9,26]],"date-time":"2026-09-26T10:08:27Z","timestamp":1790417307000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Ligand \u03c0\u2010Conjugation Area Modulates Hydrogen Evolution Performance in Metal\u2013Organic Frameworks"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3073-5166","authenticated-orcid":false,"given":"Chenxi","family":"Tan","sequence":"first","affiliation":[{"name":"Department of Chemistry National Cheng Kung University  Tainan Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2532-1380","authenticated-orcid":false,"given":"I\u2010Wen Peter","family":"Chen","sequence":"additional","affiliation":[{"name":"Department of Chemistry National Cheng Kung University  Tainan Taiwan"},{"name":"Interdisciplinary Research Center on Material and Medicinal Chemistry National Cheng Kung University  Tainan Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,9,26]]},"reference":[{"key":"e_1_2_10_2_1","doi-asserted-by":"crossref","first-page":"1026","DOI":"10.1016\/j.ijhydene.2025.01.033","article-title":"Hydrogen as an Alternative Fuel: A Comprehensive Review of Challenges and Opportunities in Production, Storage, and Transportation","volume":"102","author":"Hossain Bhuiyan M. 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