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Due to the limited availability of suitable chiral\u2010crystal materials, their unconventional superconductivity (SC) remains largely unexplored. Here, the discovery of unconventional SC in the La(Rh,Ir)Si family of materials is reported by combining muon\u2010spin spectroscopy, band\u2010structure calculations, and perturbation theory. This family, characterized by a double\u2010helix chiral structure, hosts exotic multifold fermions that are absent in other topological chiral crystals. While LaRhSi behaves as a fully\u2010gapped superconductor, the substitution of 4\n                    <jats:italic>d<\/jats:italic>\n                    \u2010Rh by 5\n                    <jats:italic>d<\/jats:italic>\n                    \u2010Ir significantly enhances the SOC and leads to the emergence of topological nodal\u2010line SC in LaIrSi. The developed model shows that the nodal\u2010line SC arises from an isotropic SOC with a specific strength. Such an exotic mechanism expands the conventional understanding of material candidates for unconventional SC, which typically rely on a significantly anisotropic SOC to promote the triplet pairing. The current\u00a0work establishes a new type of phase diagram, which provides a comprehensive roadmap for identifying and engineering unconventional SC in chiral crystals. Furthermore, it calls for renewed investigations of unconventional SC in other widely studied superconductors with a chiral\u00a0structure.\n                  <\/jats:p>","DOI":"10.1002\/adma.202511385","type":"journal-article","created":{"date-parts":[[2025,8,21]],"date-time":"2025-08-21T10:14:27Z","timestamp":1755771267000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Discovery of Nodal\u2010Line Superconductivity in Chiral Crystals"],"prefix":"10.1002","volume":"37","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5916-0020","authenticated-orcid":false,"given":"Tian","family":"Shang","sequence":"first","affiliation":[{"name":"Key Laboratory of Polar Materials and Devices (MOE), School of Physics and Electronic Science East China Normal University Shanghai 200241 China"},{"name":"Chongqing Key Laboratory of Precision Optics Chongqing Institute of East China Normal University Chongqing 401120 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Laboratory of Polar Materials and Devices (MOE), School of Physics and Electronic Science East China Normal University Shanghai 200241 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mukkattu O.","family":"Ajeesh","sequence":"additional","affiliation":[{"name":"Max Planck Institute for Chemical Physics of Solids N\u00f6thnitzer Str. 40 01187 Dresden Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Michael","family":"Nicklas","sequence":"additional","affiliation":[{"name":"Max Planck Institute for Chemical Physics of Solids N\u00f6thnitzer Str. 40 01187 Dresden Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yang","family":"Xu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Polar Materials and Devices (MOE), School of Physics and Electronic Science East China Normal University Shanghai 200241 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