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Here, we demonstrate a paradigm shift in HPL phase stability by introducing asymmetric bottlebrush block copolymers (BBCPs) with engineered architectural and conformational asymmetries. This molecular design strategy fundamentally eliminates the chain packing frustrations that have historically plagued HPL phases, yielding the stable HPL phases in bulk materials. Our approach achieves an unprecedented composition window and exceptional thermal stability up to 300\u00b0C without order\u2010to\u2010disorder transitions. Dissipative particle dynamics (DPD) simulations reveal that the synergy between backbone semi\u2010rigidity and asymmetric side chain lengths drives this remarkable stabilization. By transforming HPL phases from metastable phases into robust, readily accessible nanomaterials, this work opens new opportunities for their deployment in high\u2010performance photonic crystals, selective separation membranes, and mechanical metamaterials.<\/jats:p>","DOI":"10.1002\/anie.202523944","type":"journal-article","created":{"date-parts":[[2026,2,15]],"date-time":"2026-02-15T08:31:09Z","timestamp":1771144269000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Thermally Robust Hexagonally Perforated Lamellae Enabled by Asymmetric Bottlebrush Copolymers"],"prefix":"10.1002","volume":"65","author":[{"given":"Xiaoyu","family":"Geng","sequence":"first","affiliation":[{"name":"Tianjin Key Laboratory of Composite and Functional Materials School of Materials Science and Engineering Tianjin University  Tianjin 300350 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