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Here, we introduced a multifunctional polyamino acid interface that enhances neural interfacing by combining biocompatibility, antimicrobial activity, and antifouling properties. Applied to flexible electrodes, this coating reduces foreign body reaction and preserves neuronal proximity, ensuring stable integration with brain tissue. In chronic rodent models, functionalized electrodes achieve high\u2010fidelity single\u2010unit recordings for over 300 days with significantly higher spike amplitudes and yield than bare controls. Notably, the interface enables an order\u2010of\u2010magnitude improvement in neuromodulation efficiency, evoking robust motor responses at only 2\u00a0\u00b5A compared to 100\u00a0\u00b5A for uncoated probes. Multi\u2010omics analysis reveals a molecularly profound alteration in the host tissue response, transitioning from a pro\u2010inflammatory injury signature to an attenuated inflammatory state with improved tissue homeostasis. Furthermore, the interface's resistance to biological \u201ccementing\u201d facilitates damage\u2010free electrode removal and recovery, preserving the neural architecture and enabling the possibility of chronic replacement. This universal platform offers a promising and practical strategy for the next generation of stable, clinically viable neural\u2013computer interfaces.<\/jats:p>","DOI":"10.1002\/adma.74519","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T14:04:11Z","timestamp":1785852251000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Multifunctional Electrode\/Neural Integration Interface Enabling Chronic High\u2010Fidelity Neural Recording and an Order\u2010of\u2010Magnitude Neuromodulation Quality"],"prefix":"10.1002","volume":"38","author":[{"given":"Meiyu","family":"Shao","sequence":"first","affiliation":[{"name":"Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing 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