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However, clinical progress has been hindered by the lack of potent and structurally diverse G4\u2010targeting ligands. Herein, using parallel\n                    <jats:italic>KRAS<\/jats:italic>\n                    proximal promoter G4 (\n                    <jats:italic>KRAS<\/jats:italic>\n                    \u2010G4) as a model system, we screened an in\u2010house natural product library and identified dehydroevodiamine (DEE) as a novel G4 stabilizer. Although DEE showed only modest anticancer activity, structural analyses determined its predominant binding mode to\n                    <jats:italic>KRAS<\/jats:italic>\n                    \u2010G4. Leveraging these structural insights, we rationally designed and synthesized 15 DEE analogues. Among them, compound\n                    <jats:bold>7i<\/jats:bold>\n                    emerged as the lead candidate, demonstrating a 9\u2010fold higher binding affinity and up to 20\u2010fold improvement in antiproliferative activity over DEE. We further determined the high\u2010resolution NMR structure of the\n                    <jats:italic>KRAS<\/jats:italic>\n                    \u2010G4\u2013\n                    <jats:bold>7i<\/jats:bold>\n                    complex, uncovering a distinct dual\u2010binding mode, featuring extensive \u03c0\u2013\u03c0 stacking interactions with outer G\u2010tetrads and specific hydrogen bonding within groove regions. Functional analysis showed\n                    <jats:bold>7i<\/jats:bold>\n                    effectively suppressed transcription of several G4\u2010containing oncogenes, induced genome\u2010wide G4 formation, and triggered DNA damage in colorectal cancer cells. Moreover,\n                    <jats:bold>7i<\/jats:bold>\n                    significantly inhibited the growth of patient\u2010derived colorectal tumor organoids. Overall, our findings establish a structural framework for rational design of parallel G4\u2010targeting ligands and emphasize an alternative G4\u2010based therapeutic strategy for\n                    <jats:italic>KRAS<\/jats:italic>\n                    \u2010driven cancers.\n                  <\/jats:p>","DOI":"10.1002\/anie.8271527","type":"journal-article","created":{"date-parts":[[2026,6,7]],"date-time":"2026-06-07T16:42:24Z","timestamp":1780850544000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Structure\u2010Informed Design of Distinct Parallel G\u2010Quadruplex Stabilizers for\n                    <i>KRAS<\/i>\n                    \u2010Driven Cancer Therapy"],"prefix":"10.1002","volume":"65","author":[{"given":"Lulu","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Natural Medicines Basic Medical Research Innovation Center for Anti\u2010Cancer Drugs (Ministry of 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