The shift from traditional "sense-and-treat" to autonomous, closed-loop therapy is marked by self-decision-making bioelectronic systems, where material innovation serves as a key driver. This review highlights how advanced materials enable seamless integration of high-performance sensing, intelligent computing, and adaptive intervention. We summarize recent progress in electrochemical, electrophysiological, optical, and mechanical sensors made from soft conductors, responsive polymers, and nanocomposites, which provide reliable physiological data. The evolution from threshold-based to neuromorphic decision architectures is also discussed, translating sensor data into real-time therapeutic commands. Diverse material platforms drive functional outputs—such as precise electrical stimulation, on-demand drug delivery, mechanical actuation, and optical modulation—demonstrated in artificial pancreas systems, neural interventions, and smart wound dressings. Finally, we address system-level integration strategies and key clinical challenges, including biocompatibility, sustainable power, and regulatory translation. Through a materials-focused lens, this review outlines a roadmap for next-generation autonomous and personalized medicine.

Self-deciding medical devices that can "think" and administer treatment autonomously are moving from science fiction to reality. This review outlines the development of self-decision-making bioelectronic systems, which transform traditional "sense-then-treat" approaches into closed-loop systems that integrate real-time sensing, intelligent judgment, and precise intervention—all driven by material innovation. Key materials like conductive polymers, carbon nanomaterials, liquid metals, and biodegradable biomaterials enable flexible, biocompatible interfaces capable of efficient signal transmission. These systems monitor vital signs such as blood glucose or neural activity via electrochemical or optical methods, then process the data using threshold logic or machine learning to trigger immediate micro-scale electrical stimulation or drug delivery.

Applications range from artificial pancreas systems and smart wound dressings to deep brain stimulation, demonstrating how materials enable true interaction between devices and living organisms. For example, in diabetes management, such systems can autonomously detect blood sugar changes and release insulin; in neuroscience, implants can recognize abnormal brain signals and intervene in real time. Despite challenges in long-term stability, flexible encapsulation, and ethical regulation, the fusion of advanced materials and algorithms is paving the way for fully autonomous, personalized medicine.

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DOI: 10.1002/adma.202521164