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Despite its potency, Dox suffers from poor solubility, non\u2010specific distribution, and severe toxicity, often compromising therapeutic efficacy. Addressing these obstacles, this study explores cobalt\u2010aluminium layered double hydroxides (Co\u2010Al LDHs) as smart nanocarriers for targeted melanoma therapy. Capitalizing on their tunable structure, high drug\u2010loading capacity, and biocompatibility, Co\u2010Al LDHs facilitate enhanced encapsulation, sustained release, and selective tumor accumulation of Dox. Density Functional Theory (DFT) analyses confirm robust molecular interactions between Dox and the LDH matrix, ensuring structural stability and favorable energetics for drug delivery. In vitro assays reveal significant cytotoxicity (\u224880%) against melanoma cells and with minimal toxicity (\u22488%) to normal muscle cells. Furthermore, in vivo evaluations using luciferase\u2010tagged B16\u2010F10 melanoma models demonstrate pronounced tumor inhibition and excellent systemic biocompatibility. Augmented by machine learning\u2010guided force field modelling, this platform also offers a predictive framework for engineering next\u2010generation nanotherapeutics. Together, these findings position Co\u2010Al LDHs as a promising frontier in nanomedicine, merging targeted delivery, controlled release, and computational precision to overcome current therapeutic barriers in melanoma treatment and beyond.<\/jats:p>","DOI":"10.1002\/smll.202506499","type":"journal-article","created":{"date-parts":[[2025,9,18]],"date-time":"2025-09-18T10:57:57Z","timestamp":1758193077000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Doxorubicin Intercalated Co\u2010Al Layered Double Hydroxide Nanocarrier With pH\u2010Responsive Controlled Release and Selective Melanoma Suppression: Toward Next\u2010Generation Nanotherapeutics"],"prefix":"10.1002","volume":"21","author":[{"given":"Swapan","family":"Maity","sequence":"first","affiliation":[{"name":"School of Materials Science and Technology Indian Institute of Technology (Banaras Hindu University)  Varanasi 221005 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Akshita","family":"Upreti","sequence":"additional","affiliation":[{"name":"Department of Biological Sciences, Birla Institute of Technology and Science Pilani (K. 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