The highly intricate structures of biological systems make the precise probing of biological behaviors at the cellular‐level particularly difficult. As an advanced toolset capable of exploring diverse biointerfaces, high‐aspect‐ratio nanowires stand out with their unique mechanical, optical, and electrical properties. Specifically, semiconductor nanowires show much promise in their tunability and feasibility for synthesis and fabrication. Thus far, semiconductor nanowires have shown favorable results in deciphering biological communications and translating this cellular language through the nanowire‐based biointerfaces. In this perspective, the synthesis and fabrication methods for different kinds of nanowires and nanowire‐based structures are first surveyed. Next, several cellular‐level nanowire‐enabled applications in biophysical dynamics probing, physiological or biochemical sensing, and biological activity modulation are highlighted. Then, the progress of functionalized nanowires in drug delivery and bioenergy production is reviewed. Finally, the current limitations of nanowires and an outlook into the next generation of nanowire‐based devices at the biointerfaces are concluded.

Summary Current technological advances in neural probing and modulation have enabled an extraordinary glimpse into the intricacies of the nervous system. Particularly, nanomaterials are proving to be an incredibly versatile platform for neurological applications owing to their biocompatibility, tunability, highly specific targeting and sensing, and long-term chemical stability. Among the most desirable nanomaterials for neuroengineering, freestanding nanomaterials are minimally invasive and remotely controlled. This review outlines the most recent developments of freestanding nanomaterials that operate on the neuronal interface. First, the different nanomaterials and their mechanisms for modulating neurons are explored to provide a basis for how freestanding nanomaterials operate. Then, the three main applications of subcellular neuronal engineering—modulating neuronal behavior, exploring fundamental neuronal mechanism, and recording neuronal signal—are highlighted with specific examples of current advancements. Finally, we conclude with our perspective on future nanomaterial designs and applications.

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