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However, their adoption in aerogel fabrication is limited by material and structure\u2010performance deficiencies (e.g., hydrophilicity, low surface area, brittleness, limited tactile tailorability). Nevertheless, stereocomplexation, or co\u2010crystallization between polymeric enantiomers, offers a pathway toward overcoming such limitations. Herein, stereocomplexation is used to fabricate poly(lactide) (PLA)\u2010based aerogels, with stereocomplex crystals (SCs) assembling into a highly ordered morphology\/topology within aerogel precursors. To tailor aerogel bulk properties, a blending approach is implemented during sol\u2013gel processing, leading to sequential crystallization of sol\u2013gel system constituents. This pathway yields hierarchically macro\u2010\/meso\u2010porous aerogels (\n                    <jats:italic>S<\/jats:italic>\n                    <jats:sub>BET<\/jats:sub>\n                    up to \u223c186\u00a0m\n                    <jats:sup>2<\/jats:sup>\n                    \u00b7g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), offering a variety of superstructures that resemble cuticular plant tissue. These aerogels resist brittle failure under compression (70% strain) and withstand cyclic loading (100 cycles, 20% strain) without significant densification. Such aerogels also exhibit functional properties including superhydrophobicity\/superoleophilicity and are well\u2010suited for continuous oil\u2013water separation. Additionally, fantastic geometric\u2010thermal stability, insulation\/heat dissipation ability (\n                    <jats:italic>k<\/jats:italic>\n                    <jats:sub>Cond<\/jats:sub>\n                    \u00a0\u223c36\u00a0mW\u00b7m\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00b7K\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), and phase\u2010change insulation characteristics are achieved. These functionalities arise from multi\u2010scale structural features and demonstrate how coupling stereocomplexation and sequential crystallization offers pathways to construct intricate superstructure morphologies\/topologies, and overcome material\/structure\u2010performance limitations in green aerogels.\n                  <\/jats:p>","DOI":"10.1002\/adma.75136","type":"journal-article","created":{"date-parts":[[2026,9,29]],"date-time":"2026-09-29T08:03:17Z","timestamp":1790668997000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["A Thermoreversible Gelation Pathway to Plant Cuticle\u2010Inspired Biopolymer Aerogel Monoliths Based on Network\u2010Spherulitic Crystal Assemblies"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5771-1629","authenticated-orcid":false,"given":"Anthony V.","family":"Tuccitto","sequence":"first","affiliation":[{"name":"Multifunctional Composites Manufacturing 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