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However, the relationship between the interlayer architecture, molecular configuration of aromatic cations, and resulting stability remains poorly understood. Herein, we systematically investigate phenyl alkylammonium\u2010based RP 2D perovskites with varying alkyl chain lengths (\u2500(CH\n                    <jats:sub>2<\/jats:sub>\n                    )\n                    <jats:sub>m<\/jats:sub>\n                    NH\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>+<\/jats:sup>\n                    with m = 1\u20134) of organic cations. We find that odd\u2010carbon cations (m = 1, 3) preferentially form type\u2010I 2D perovskites featuring interdigitated organic cations, which induces substantial inorganic distortion and lower octahedral symmetry to the\n                    <jats:italic>C<\/jats:italic>\n                    <jats:sub>1<\/jats:sub>\n                    point group. Even\u2010carbon cations (m = 2, 4) favor type\u2010II 2D perovskites with well\u2010defined interlayer gaps, wherein the alkylammonium groups rotate to optimize registry with the inorganic sublattice, minimizing distortion and yielding higher\u2010symmetry\n                    <jats:italic>\n                      D\n                      <jats:sub>2<\/jats:sub>\n                    <\/jats:italic>\n                    <jats:sub>h<\/jats:sub>\n                    octahedra. Furthermore, we demonstrate that intrinsic structural stability of RP 2D perovskites is primarily governed by \u03c0\u2013\u03c0 packing within the organic layer, whereas air stability of the thin films is determined by surface hydrophobicity. The type\u2010II films exhibit higher hydrophobicity, conferring enhanced stability under ambient conditions compared to type\u2010I films. These findings establish odd\u2010even alkyl chain parity as a design principle for tailoring structurally diverse yet stable RP 2D perovskites.\n                  <\/jats:p>","DOI":"10.1002\/anie.6772439","type":"journal-article","created":{"date-parts":[[2026,8,29]],"date-time":"2026-08-29T04:53:52Z","timestamp":1787979232000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Odd\u2010Even Alkyl Chain Effect of Aromatic Monoammoniums on the Interlayer Architecture and Stability of Ruddlesden\u2013Popper 2D Perovskites"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-3959-0795","authenticated-orcid":false,"given":"Yang","family":"Liu","sequence":"first","affiliation":[{"name":"Ningbo Key Laboratory of Electronic Materials and Equipment School of Materials and Energy Engineering NingboTech University  Ningbo 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-5366-4675","authenticated-orcid":false,"given":"Jiaxing","family":"Song","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Advanced Tandem Photovoltaic Technology College of Biological and Chemical Engineering Jiaxing University  Jiaxing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6609-4028","authenticated-orcid":false,"given":"Zaifang","family":"Li","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Advanced Tandem Photovoltaic Technology College of Biological and Chemical Engineering Jiaxing University  Jiaxing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9013-6934","authenticated-orcid":false,"given":"Jifeng","family":"Wu","sequence":"additional","affiliation":[{"name":"KAUST Catalysis Center (KCC) Division of Physical Science and Engineering King Abdullah University of Science and Technology (KAUST)  Thuwal Saudi Arabia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bin","family":"Fan","sequence":"additional","affiliation":[{"name":"Kunshan GCL Optoelectronic Co., Ltd  Kunshan Jiangsu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2418-9210","authenticated-orcid":false,"given":"Wei","family":"Chen","sequence":"additional","affiliation":[{"name":"Wuhan National Laboratory for Optoelectronics School of Optical and Electronic Information Huazhong University of Science and Technology  Wuhan Hubei China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-3927-7054","authenticated-orcid":false,"given":"Qiuju","family":"Liu","sequence":"additional","affiliation":[{"name":"Kunshan GCL Optoelectronic Co., Ltd  Kunshan Jiangsu 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